Weixin Guan’s research while affiliated with University of Texas at Austin and other places

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Publications (23)


Material-to-system tailored multilayer-cyclic strategy toward practical atmospheric water harvesting
  • Article

May 2025

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2 Reads

Proceedings of the National Academy of Sciences

Yaxuan Zhao

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Weixin Guan

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Yan Zhe Wong

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[...]

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Guihua Yu

Solar-driven atmospheric water harvesting (AWH) presents a sustainable approach for freshwater production with sunlight as the sole energy input. To address challenges posed by diurnal moisture variations and diffusive sunlight, we present a system-wide approach that synergistically enhances moisture capture and solar energy utilization in an integrated water harvester. Moisture utilization at the bulk sorbent scale is improved through the hierarchical pore structure of scalable biomass gel sheets enabling rapid regeneration and is further upscaled to system-level performance through a kinetics-matched, continuously multicyclic operation protocol in a multilayered device. Solar energy utilization is enhanced by thermoresponsive hydrogels that lower the energy threshold for water desorption and by efficient thermal and mass flow management that increases energy efficiency. Our system delivers up to 235.09 mL d ⁻¹ of water with an energy efficiency as high as 26.4%, excluding solar panel power. This work offers an insight into developing energy-, material-, and space-efficient AWH systems from a cross-scale understanding of sorbent properties, device engineering, and operation protocol tailoring.


Essential inputs (water, fertilizer, pesticide) for plant growth cycle.
Core properties of hydrogels determined by structure, tunability, and physicochemical characteristics; key attributes include swelling, controlled release, and conductivity for agricultural applications.
Smart hydrogels for agrochemical release. (A), Schematic diagram of NPK fertilizer release mechanism. (B), release behavior of nitrogen (N) and phosphorus (P) in soil over 30 days. (A, B), Reproduced with permission: Copyright 2024, Elsevier [21]. (C), Schematic diagram of the fabrication of multi‐responsive hydrogel system. (D), Release behavior of insecticide under varying conditions, focusing on temperature, pH, and enzymatic action. (C, D), Reproduced with permission: Copyright 2022, American Chemical Society [22].
Smart hydrogels for self‐irrigation. (A), Schematic illustration of water capturing/releasing and moisture absorption by SMAG. Reproduced with permission: Copyright 2019, Wiley‐VCH GmbH [38]. (B), Schematic diagram of water absorption/release and fertilizer release operating in a diurnal cycle for SISRH. (C), SISRH performance for fertilizer release in different RH conditions. (D), Comparison of SISRH‐soil and sandy‐soil in plant growth and survival rate. (B–D), Reproduced with permission: Copyright 2024, American Chemical Society [39].
Smart hydrogel‐based sensor. (A), Energy conversion process of hydrogel‐based TENG through cyclic contact‐release and application in LED powering. B, Growth rate differences in the control group and LED treatment group. (B, C), Reproduced with permission: Copyright 2021, Elsevier [47]. (C), Schematic illustration of the portable hydrogel electrode for ATZ detection. (D), Comparison of ATZ residues in lake water and farmland soil by HPLC and hydrogel‐based portable sensor. (C, D), Reproduced with permission: Copyright 2024, American Chemical Society [48].

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Smart Hydrogels for Sustainable Agriculture
  • Article
  • Full-text available

April 2025

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97 Reads

The growing global population, coupled with increasing food demand and water scarcity, has intensified the need for advancements in modern agriculture. As an emerging class of materials featured by intensively tunable properties, smart hydrogels offer innovative solutions to challenges associated with conventional agricultural practices, such as excessive agrochemical and water use and inefficiencies that contribute to environmental degradation. Additionally, hydrogel‐based sensors can monitor environmental conditions and crop health, enabling precise adjustments to optimize growth and resource use. By serving as platforms for the slow and controlled delivery of agrochemicals and smart sensors, hydrogel systems can enhance resource efficiency, reduce labor demands, and improve crop yields in an environmentally sustainable manner. This Perspective article summarizes recent advancements in hydrogel‐based materials, highlights existing challenges, and proposes potential research directions, with a focus on developing advanced hydrogel systems to transform agricultural practices. image

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Molecular functionalization strategy of natural polysaccharides as hydrogel sorbents. Molecular functionalization of natural polysaccharides, derived from abundant biomass, enhances their water uptake and lowers the desorption temperature, activating them as SAWH sorbents. At room temperature, the hydrogel absorbs moisture and swells, representing the water sorption state (blue swollen hydrogel, upper right). Upon heating, hydrophobic interactions among the thermoresponsive groups dominate, causing the hydrogel network to contract and transition to the water release state (red contracted hydrogel, bottom right).
Synthesis and properties of ZHPC. a) Schematic representation of the synthetic route for molecularly functionalized cellulose in AWH application. The chemical structure depicted is for illustrative purposes only. b) ¹H NMR spectra illustrating HPC, ZHPC−1, ZHPC−2, and ZHPC−3, along with the chemical structure of ZHPC. c) FTIR spectra comparison of pristine cellulose, HPC, ZHPC−3, and the zwitterionic agent (3‐((3‐chloropropyl)dimethylammonio)propane‐1‐sulfonate). d) XRD patterns for pristine cellulose and ZHPC−3 hydrogel. e) Swelling ratios of cellulose hydrogel and ZHPC−3 hydrogel in varied LiCl concentration solutions. f) Heat flow profiles from DSC test, showcasing the phase transition behavior of HPC, ZHPC−1, ZHPC−2, and ZHPC−3.
AWH performance of ZHPC hydrogel sorbents. a) Static water vapor sorption‐desorption curves for ZHPC−1, ZHPC−2, and ZHPC−3/LiCl hydrogel sorbents at 30% RH and 25 °C. Desorption conditions: 60 °C, 15% RH. b) Static water vapor sorption‐desorption curves of ZHPC−3/LiCl hydrogel sorbents at 15%, 30%, and 60% RH at 25 °C. Desorption conditions: 60 °C, 15% RH. c) Heat flow profiles detailing the evaporation behavior of cellulose hydrogel and ZHPC−3/LiCl hydrogel. d) Static desorption curves of ZHPC−3/LiCl hydrogel under various temperatures with a consistent water vapor pressure of 3.17 kPa. e) Cycling performance of ZHPC−3/LiCl hydrogel over an extended period with repeated sorption‐desorption cycles; sorption at 30% RH and desorption at 60 °C. f) Static water vapor sorption‐desorption curves of ZHPC−3/LiCl hydrogel pre‐ and post‐cycling. g) Water uptake and water collection at varying RH levels. h) Cycling test for water collection using ZHPC−3/LiCl hydrogel at 30% RH.
Material properties and AWH performance of ZHBS and ZHBC hydrogel sorbents. Panels (a–e) depict the starch system (ZHBS), and f–j) the chitosan system (ZHBC), with mirrored analyses. a,f) ¹H NMR spectra show HBS/HBC, ZHBS/ZHBC−1, and ZHBS/ZHBC−2, including their chemical structures. b,g) XRD patterns compare pristine substrates with ZHBS/ZHBC‐1, illustrating structural transitions. c,h) DSC heat flow profiles reveal phase transition behaviors across HBS/HBC, ZHBS/ZHBC−1, and ZHBS/ZHBC−2. d,i) Static water vapor sorption‐desorption curves at 15%, 30%, and 60% RH at 25 °C, with desorption at 60 °C, 15% RH, for ZHBS/ZHBC−1 LiCl hydrogels. e,j) Cycling performance over extended periods, with sorption at 30% RH and desorption at 60 °C, for ZHBS/ZHBC−1 LiCl hydrogels.
Outdoor AWH test. a) Display of a series of bottles containing large‐volume 2 wt.% ZHPC solution, illustrating the scalability of the synthesis process. b) Water collection device setup. Scale bar: 10 cm. The inset at the top right shows the ZHPC hydrogel sorbent, with a diameter of ≈15 cm and a thickness of ≈2 cm. The bottom right inset shows water droplets condensed on the device's cover. c) Displays the water content from sorption/desorption processes and the accumulated water collected from condensation at the top, with outdoor temperature and RH data shown at the bottom. The light blue and red regions indicate the sorption and desorption phases, respectively. These measurements were taken on March 1st−6th, 2024, in Austin, Texas, USA. d) The photograph of the collected water. e) ICP‐MS analysis detailing cation residues in the collected water. Lithium lacks a guideline level in drinking water. An estimated threshold of 0.70 mg L⁻¹ is based on the EPA's oral reference dose of 20 µg kg⁻¹ day⁻¹.[⁴⁴] f) Comparative analysis of different materials based on key intrinsic properties essential for practical AWH applications.
Molecularly Functionalized Biomass Hydrogels for Sustainable Atmospheric Water Harvesting

February 2025

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265 Reads

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2 Citations

Atmospheric water harvesting (AWH) offers a promising pathway to alleviate global water scarcity, highlighting the need for environmentally responsible sorbent materials. In this context, this research introduces a universal strategy for transforming natural polysaccharides into effective hydrogel sorbents, demonstrated with cellulose, starch, and chitosan. The methodology unites alkylation to graft thermoresponsive groups, thereby enhancing water processability and enabling energy‐efficient water release at lower temperatures, with the integration of zwitterionic groups to ensure stable and effective water sorption. The molecularly functionalized cellulose hydrogel, exemplifying our approach, shows favorable water uptake of 0.86–1.32 g g⁻¹ at 15–30% relative humidity (RH), along with efficient desorption, releasing 95% of captured water at 60 °C. Outdoor tests highlight the water production rate of up to 14.19 kg kg⁻¹ day⁻¹ by electrical heating. The proposed molecular engineering methodology, which expands the range of raw materials by leveraging abundant biomass feedstock, has the potential to advance sorbent production and scalable AWH technologies, contributing to sustainable solutions.


Schematic illustration of the HEA iNPs and HESA NCs synthesis
a Colloidal synthesis of HEA iNPs starts with homogeneous nucleation of metal atoms connected by metallic bonds, followed by the growth of nuclei into NPs. After an oxidative etching process, the HEA NPs are supposed to deliver an irregular shape due to the random etching of surface atoms. b In the case of HESA NCs, the MESA nanocubes are firstly formed via ligand exchange and cyano polymerization, followed by selective etching of the internal space, generating HESA NCs.
Synthesis and characterizations of MESA nanocubes and HESA NCs
a BF-TEM image and SAED pattern of MESA nanocubes. Scale bar is 2 1/nm. b HAADF-STEM of an individual MESA nanocube. c Fe-L-edge EELS throughout the MESA nanocube. d EDS line scans of an individual MESA nanocube. e BF-TEM image and SAED pattern of HESA NCs. Scale bar is 2 1/nm. f HAADF-STEM of an individual HESA NC. g zoom-in HAADF-STEM image and localized Fe-L-edge EELS on the corner and wall of the HESA NC, respectively. h EDS line scans of an individual HESA NC. EDX elemental maps of an individual MESA nanocube (i) and HESA NC (j). Scale bars are 50 nm for all images. k PXRD patterns of MESA nanocubes (black line) and HESA NCs (red line). Red dashed lines: FeCo PBA (JCPDS: #46-0907).
Structural analysis and formation mechanistic study of HESA NCs
a XPS spectra of Fe 2p of gel samples before and after the etching process. b Fe K-edge XANES spectra of Fe foil, FeO, Fe2O3, and gel samples before and after the etching process. c FT k²-weighted χ(k) function of EXAFS spectra for the Fe K-edge. d Atomic percentage of metal elements and corresponding ∆S after etching MESA nanocubes by ammonia with concentration of 0 (E0), 2 (E1), 5 (E2), 10 (E3), 15 (E4), and 20 (E5) mmol. ATR-FTIR localized spectra (e) and PXRD patterns (f) of the etched products. g Schematic illustration of the lattice evolution during the etching process with localized dissolution of [Fe(III)(CN)6]³⁻ and increasing ∆S via the ligand substitution mechanism.
Electrocatalytic NO3RR performance
a Linear scan voltammetry curves of Fe-HESA NCs and Fe-Co NCs normalized to the geometric area. b MA and TOF for NH3 production at various potentials. c FE of NH3 over Fe-HESA NCs (blank pattern) and Fe-Co NCs (slash pattern) at different potentials. d YR of NH3 over Fe-HESA NCs and Fe-Co NCs at different potentials. All potentials are not iR corrected. e¹H NMR spectrum of the products generated during the electrocatalytic NO3RR over Fe-HESA NCs in 0.1 M Na¹⁵NO3 or 0.1 M Na¹⁴NO3 at −0.6 VRHE. f Quantification of NH3 via UV-Vis and NMR measurements at −0.6 V vs. RHE. g Long-term chronoamperometry test for 150 h and the cycling test (inset) at −0.6 VRHE. Error bars denote the standard deviations calculated from three independent measurements.
Mechanistic investigation of the NO3RR on HESA NCs
Operando SR-FTIR signals in the range of 4000–2800 cm⁻¹ (a) and 2200–1000 cm⁻¹ (b). c IR peak intensity versus the applied potential for the NO3RR process. d Conceptional illustration of the effects of configurational entropy and lattice symmetry on electronic property. The electron localization increases with increasing entropy and decreasing symmetry.
General synthesis of high-entropy single-atom nanocages for electrosynthesis of ammonia from nitrate

August 2024

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91 Reads

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26 Citations

Given the growing emphasis on energy efficiency, environmental sustainability, and agricultural demand, there’s a pressing need for decentralized and scalable ammonia production. Converting nitrate ions electrochemically, which are commonly found in industrial wastewater and polluted groundwater, into ammonia offers a viable approach for both wastewater treatment and ammonia production yet limited by low producibility and scalability. Here we report a versatile and scalable solution-phase synthesis of high-entropy single-atom nanocages (HESA NCs) in which Fe and other five metals-Co, Cu, Zn, Cd, and In-are isolated via cyano-bridges and coordinated with C and N, respectively. Incorporating and isolating the five metals into the matrix of Fe resulted in Fe-C5 active sites with a minimized symmetry of lattice as well as facilitated water dissociation and thus hydrogenation process. As a result, the Fe-HESA NCs exhibited a high selectivity toward NH3 from the electrocatalytic reduction of nitrate with a Faradaic efficiency of 93.4% while maintaining a high yield rate of 81.4 mg h⁻¹ mg⁻¹.



Chemistries and materials for atmospheric water harvesting

June 2024

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91 Reads

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27 Citations

Chemical Society Reviews

Atmospheric water harvesting (AWH) is recognized as a crucial strategy to address the global challenge of water scarcity by tapping into the vast reserves of atmospheric moisture for potable water supply. Within this domain, sorbents lie in the core of AWH technologies as they possess broad adaptability across a wide spectrum of humidity levels, underpinned by the cyclic sorption and desorption processes of sorbents, necessitating a multi-scale viewpoint regarding the rational material and chemical selection and design. This Invited Review delves into the essential sorption mechanisms observed across various classes of sorbent systems, emphasizing the water-sorbent interactions and the progression of water networks. A special focus is placed on the insights derived from isotherm profiles, which elucidate sorbent structures and sorption dynamics. From these foundational principles, we derive material and chemical design guidelines and identify key tuning factors from a structural-functional perspective across multiple material systems, addressing their fundamental chemistries and unique attributes. The review further navigates through system-level design considerations to optimize water production efficiency. This review aims to equip researchers in the field of AWH with a thorough understanding of the water-sorbent interactions, material design principles, and system-level considerations essential for advancing this technology.


Design of bistable eletrochromic systems based on supramolecular interactions. a) The components and 3D network interpenetrating structure of EC ionic hydrogel. b) Sketch depicting interfacial delamination in bistable electrochromic devices and the confinement of EC components induced by supramolecular interactions. c) The EC mechanisms involved in the system.
Feasibility of the bistable electrochromic systems based on the supramolecular interactions. a) Absorption spectra of amylose (0.1 mol L⁻¹ for glucose units), KI (0.05 mol L⁻¹) and a mixture of KI (0.05 mol L⁻¹), amylose (0.1 mol L⁻¹ for glucose units) before and after voltage stimulation. b) The ionic gel exhibits colored and colorless states when combined with KI/amylose and KI3/amylose, respectively. c) SEM image of PDMAEA ionic gel. d) Diffusion of the EC components in liquid device. e) Supramolecular interactions within the EC gel device induce confinement of the ionic gel among EC components. f) Infrared absorption spectra of the mixtures of KI and PDMAEA, KI3 and PDMAEA, and PDMAEA alone. g) The XPS spectra of oxidized KI and the mixture of oxidized KI and PDMAEA under the positive voltage stimulation. h) Raman spectra of amylose, the mixture of KI, PDMAEA and amylose under the voltage of 1.5 V.
Electrochromic properties. a) The architecture of the device. b) The chemical structure of PAM, PDMAEA, PDMAPS. c) The transmittance changes and decay ratio over 20 min of devices containing hydrogel, cationic gel, and zwitterionic gel. d) The ion diffusion process and related electrostatic interactions between gels and ions in the EC system. e) Ion diffusion across various gels was monitored through absorption spectra at 350 nm. (Inset: device for in situ monitoring of ion diffusion). f) The transmittance changes and decay ratio of devices containing different ratios of KI and Glucose (subunit of amylose). g) The transmittance changes and decay ratio of devices containing different concentrations of KI and amylose. h) The swelling ratio of hydrogels with different contents of cross‐linkers. i) The transmittance changes and decay ratio of devices containing hydrogels with different contents of cross‐linkers.
Electrochromic performance and application of the gel‐state device a) The open voltage of the device. b) Full spectra change of the device under different voltage stimulations. c) The maximum transmittance variations of different reported bistable EC systems. d) Stimulation voltage (top) and transmittance (bottom) of the device under stimulation of +1.9 V for 16 s, power off for 2 h, −1.2 V for 21 s at 610 nm. e) Demonstration of the flexible EC display. f) The power consumption of the developed display, under a voltage of 1.9 V 16 s and −1.2 V 21 s, during the display of static images for 7200 s, is compared with that of previously reported transparent displays.[23,24] g) The cost of various EC systems.
Bistable Electrochromic Ionogels via Supramolecular Interactions for Energy‐Efficient Displays

May 2024

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91 Reads

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12 Citations

Bistable electrochromic (EC) materials and systems offer significant potential for building decarbonization through their optical modulation and energy efficiency. However, challenges such as limited design strategies and bottlenecks in cost, fabrication, and color have hindered the full commercialization of energy‐saving EC windows and displays, with few materials achieving true bistability. Herein, a novel strategy for designing bistable electrochromic materials is proposed by leveraging supramolecular interactions. These interactions facilitate reversible color transitions, stabilize the colored structure, and enable spatial confinement to inhibit diffusion, thereby achieving bistable electrochromism. The mechanisms and materials underlying these unconventional electrochromic systems are substantiated through detailed characterization. This strategy enables the preparation of low‐cost and sustainable transparent electrochromic displays with high performance. Notably, the display information remains clearly visible for more than 2 h without consuming energy. Involving biomass materials and removable device structures also enhances the sustainability and scalability of EC technology applications and development. These results demonstrate the crucial role of supramolecular chemistry in the development of cutting‐edge materials for applications such as energy‐saving smart windows.


Fig. 1. EC mechanism and reaction process based on host-guest interaction. (A) Dynamic host-guest interactions for EC system containing simple biochemical building blocks. Amylose and cyclodextrin materials can be extracted from corn/potato by a simple repeated dissolution-centrifugation process. (B) Schematic illustration of related EC mechanism and involved EC device based on dynamic host-guest interaction. (The pore structure represents host molecules, such as, amylose, cyclodextrins, and so on. Black spheres represent carbon atoms; Blue spheres represent oxygen atoms; White spheres represent hydrogen atoms).
Fig. 2. Investigation of the EC mechanism based on dynamic host-guest interaction. (A) Absorption spectra of KI (1.0 × 10 −4 mol/L), amylose (1.0 × 10 −4 mol/L), KI 3 (1.0 × 10 −4 mol/L), amylose/KI (1.0 × 10 −3 mol/L/1.0 × 10 −4 mol/L), amylose/KI 3 (1.0 × 10 −3 mol/L/1.0 × 10 −4 mol/L), and amylose/KI 3 /Na 2 S 2 O 3 (1.0 × 10 −3 mol/L/1.0 × 10 −4 mol/L/1.0 × 10 −4 mol/L) in water. (Inset) digital photograph of aqueous solutions containing amylose (1.0 × 10 −3 mol/L) for N1, amylose/KI (1.0 × 10 −3 mol/L/1.0 × 10 −4 mol/L) for N2, amylose/KI 3 (1.0 × 10 −3 mol/L/1.0 × 10 −4 mol/L) for N3, and amylose/KI 3 /Na 2 S 2 O 3 (1.0 × 10 −3 mol/L/1.0 × 10 −4 mol/L/1.0 × 10 −3 mol/L) for N4. (B) Cyclic voltammograms of KI (2.0 × 10 −3 mol/L), amylose (2.0 × 10 −3 mol/L), and amylose/KI (2.0 × 10 −3 mol/L/2.0 × 10 −3 mol/L). (C) Absorption spectra of KI (1.0 × 10 −4 mol/L), amylose (2.0 × 10 −4 mol/L), and KI/amylose (1.0 × 10 −4 mol/L/2.0 × 10 −4 mol/L) before and after voltage stimulation. (D) Infrared absorption (IR) spectra of the mixture of amylose and KI 3 , the mixture of KI and amylose under the voltage of 1.5 V, amylose, KI 3 . (E) 1 H-NMR spectra (400 MHz, Dimethyl sulfoxide-d 6 ) of clathrates with different ratios of amylose and oxidized KI. (F) X-ray powder diffraction (XRD) of amylose, amylose and KI 3 , the mixture of KI and amylose under the voltage of 1.5 V. (G) Absorption spectra of mixture of oxidized KI and amylose (1.0 × 10 −4 mol/L/2.0 × 10 −3 mol/L), mixture of oxidized KI and HPC (1.0 × 10 −4 mol/L/2.0 × 10 −3 mol/L) and oxidized KI (1.0 × 10 −4 mol/L) in water. (Inset) digital photograph of aqueous solutions containing the mixture of oxidized KI and amylose (M1), mixture of oxidized KI and HPC (M2), and oxidized KI (M3). (H) Raman spectra of amylose, the mixture of KI and amylose under the voltage of 1.5 V. (I) The XPS spectra of the KI and the mixture of KI and amylose under the positive voltage stimulation. The concentrations for HPC and amylose polymer refer to the concentrations of glucose units.
Fig. 3. EC device optimization. (A) Schematic of an EC device. (B) Schematic illustration of the ion and electron transfer involved in the tinting and color fading process. (C) Plots of the peak current densities of KI and amylose/KI versus the square root of the scan rates. (D) Transmittance (at 630 nm) of the KI/amylose (0.04 mol/L/0.08 mol/L) in the EC device under the voltage of 1.9 V/−0.9 V. (E) Transmittance of the EC device containing different ratios of KI/glucose (subunit in amylose) under the voltage of 1.9 V/−0.9 V. (F) Transmittance of the EC device containing different concentrations of KI with the ratio of 1:2 for KI/glucose (subunit in amylose) under the voltage of 1.9 V/−0.9 V. (G) Transmittance of the EC device containing different thicknesses of the EC layers under the voltage of 1.9 V/−0.9 V. (H) Transmittance of the EC device containing different electrolytes under the voltage of 1.9 V/−0.9 V. (I) Radius and diffusion coefficient for different hydrated cations in aqueous solution.
Fig. 4. EC device characteristics. (A) Different grayscale displays with different voltage stimulations. (B) Transmittance spectra of the optimized EC device under different voltage stimulations. (C) Transmittance changes of different reported EC systems. (45-48) (D) Transmittance change of the EC device under the voltage of 1.9 V/−0.9V with different irradiation time of UV light. (E) CE of the EC system. (F) Reversibility of the device under the voltage of 1.9 V/−0.9 V. (G) CE of the EC device by reusing different times of the involved ITO electrode and ion-conducting film. (H) The sustainability characteristics of different current EC systems.
Sustainable, low-cost, high-contrast electrochromic displays via host–guest interactions

April 2024

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87 Reads

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6 Citations

Proceedings of the National Academy of Sciences

Electrochromic (EC) displays with electronically regulating the transmittance of solar radiation offer the opportunity to increase the energy efficiency of the building and electronic products and improve the comfort and lifestyle of people. Despite the unique merit and vast application potential of EC technologies, long-awaited EC windows and related visual content displays have not been fully commercialized due to unsatisfactory production cost, durability, color, and complex fabrication processes. Here we develop a unique EC strategy and system based on the natural host and guest interactions to address the above issues. A completely reusable and sustainable EC device has been fabricated with potential advantages of extremely low cost, ideal user-/environment friendly property, and excellent optical modulation, which is benefited from the extracted biomass EC materials and reusable transparent electrodes involved in the system. The as-prepared EC window and nonemissive transparent display also show comprehensively excellent properties: high transmittance change (>85%), broad spectra modulation covering Ultraviolet (UV), Visible (Vis) to Infrared (IR) ranges, high durability (no attenuation under UV radiation for more than 1.5 mo), low open voltage (0.9 V), excellent reusability (>1,200 cycles) of the device’s key components and reversibility (>4,000 cycles) with a large transmittance change, and pleasant multicolor. It is anticipated that unconventional exploration and design principles of dynamic host–guest interactions can provide unique insight into different energy-saving and sustainable optoelectronic applications.


Sustainable and Rapid Water Purification at the Confined Hydrogel Interface

January 2024

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125 Reads

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18 Citations

Emerging organic contaminants in water matrices have challenged ecosystems and human health safety. Persulfate‐based advanced oxidation processes (PS‐AOPs) have attracted much attention as they address potential water purification challenges. However, overcoming the mass transfer constraint and the catalyst's inherent site agglomeration in the heterogeneous system remains urgent. Herein, the abundant metal‐anchored loading (≈6–8 g m⁻²) of alginate hydrogel membranes coupled with cross‐flow mode as an efficient strategy for water purification applications is proposed. The organic flux of the confined hydrogel interfaces sharply enlarges with the reduction of the thickness of the boundary layer via the pressure field. The normalized property of the system displays a remarkable organic (sulfonamides) elimination rate of 4.87 × 10⁴ mg min⁻¹ mol⁻¹. Furthermore, due to the fast reaction time (<1 min), cross‐flow mode only reaches a meager energy cost (≈2.21 Wh m⁻³) under the pressure drive field. It is anticipated that this finding provides insight into the novel design with ultrafast organic removal performance and low techno‐economic cost (i.e., energy operation cost, material, and reagent cost) for the field of water purification under various PS‐AOPs challenging scenarios.


Fig. 1. AWH process and design rationale of AWH sorbents. (A) Illustration of a typical SAWH process. (B) Schematic representation of two moisture capture mechanisms: 1) Salt Deliquescence-a three-step process involving hygroscopic salts, including chemisorption, crystallization, and deliquescence, which requires elevated temperatures for complete desorption of salt hydrates; 2) Confined Hydration-molecularly confined hygroscopic sites enable water capture within the molecular mesh, allowing for water release at lower temperatures due to conformational changes in the thermoresponsive gel network without the involvement of crystal hydrates. (C) Qualitative comparison of salt-contained sorbents, highlighting key performance factors for AWH sorbents.
Fig. 2. Basic properties and characterization of copolymer hydrogels. (A) Schematic representation of copolymer structure and composition. (B) FT-IR spectra for monomers and copolymer. (C) XRD patterns of TZMG with varying copolymerization ratios. (D) Swelling ratios of hydrogels in 4 M LiCl solution. (E) Phase transition temperatures of hydrogels with different copolymerization ratios.
Fig. 3. AWH performance of TZMGs. (A) Schematic representation of the inverse mini-emulsion polymerization process, alongside SEM images and elemental mapping of as-prepared TZMG. (Scale bar: 50 μm.) (B) Water uptake of TZMGs at various RH levels. (C) Static water vapor sorption-desorption performance at different RH for TZMG-1.0. Sorption was conducted at 25 °C, while desorption took place at 60 °C. (D) Desorption curves for TZMG-1.0 at different temperatures. (E) Evaporation behavior of TZMGs and pure LiCl, hydrated with 1 g g −1 water uptake. (F) Cycling performance of TZMG-1.0, with sorption conditions set at 60% RH and a desorption temperature of 60 °C. For all tests, desorption occurred at a consistent water vapor pressure of 3.17 kPa. (G) Comparison plots of desorption performance of TZMG-1.0 with reported salt-contained/gel-based evaporation-based materials (11, 12, 26, 30, 33, 40-49). The fuchsia and turquoise dots refer to the desorption performance of this work.
Fig. 4. Photothermal ability and solar-driven vapor sorption-desorp tion properties of PZMGs. (A) Schematic illustration of the PZMG synthesis process. (Scale bar: 1 cm.) (B) UV-Vis-NIR spectra of PZMGs with varying Ppy contents, and the normalized spectral solar irradiance density of air mass 1.5 global (AM 1.5 G) tilt solar spectrum. Specifically, PZMG 1 to 4 corresponds to PZMG with 15 vol%, 10 vol%, 5 vol%, and 2 vol% of 0.1 g/mL Ppy:PSS solution. (C) Time-dependent surface temperature and the IR thermal images of PZMG-1 under different light intensities. (D) Water vapor sorption curve under 60% RH and desorption curve under 1 sun of PZMG-1, and sorption-desorption rates (green dots) of PAMG-1.
Fig. 5. Atmospheric water extraction. (A) Optical images of the homemade solar-driven AWH system. (B) Water uptake and release at different RH levels. (C) Cycling performance of PZMG at 60% RH. (D) Collected water quality assessed by ICP-MS. An estimated limit of 0.70 mg/L in drinking water was calculated by using a United States Environmental Protection Agency oral reference dose of 20 μg/kg/day (52).
Molecularly confined hydration in thermoresponsive hydrogels for efficient atmospheric water harvesting

September 2023

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314 Reads

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31 Citations

Proceedings of the National Academy of Sciences

Water scarcity is a pressing global issue, requiring innovative solutions such as atmospheric water harvesting (AWH), which captures moisture from the air to provide potable water to many water-stressed areas. Thermoresponsive hydrogels, a class of temperature-sensitive polymers, demonstrate potential for AWH as matrices for hygroscopic components like salts predominantly due to their relatively energy-efficient desorption properties compared to other sorbents. However, challenges such as limited swelling capacity due to the salting-out effect and difficulty in more complete water release hinder the effectiveness of conventional hydrogel sorbents. To overcome these limitations, we introduce molecularly confined hydration in thermoresponsive hydrogels by employing a bifunctional polymeric network composed of hygroscopic zwitterionic moieties and thermoresponsive moieties. Here, we show that this approach ensures stable water uptake, enables water release at relatively low temperatures, and exhibits rapid sorption–desorption kinetics. Furthermore, by incorporating photothermal absorbers, the sorbent can achieve solar-driven AWH with comparable water release performance. This work advances the design of AWH sorbents by introducing molecularly confined hydration in thermoresponsive hydrogels, leading to a more efficient and sustainable approach to water harvesting. Our findings offer a potential solution for advanced sorbent design with comprehensive performance to mitigate the freshwater crisis.


Citations (21)


... Besides, efficient vapor transfer and condensation can empower SDIE for a wide range of functionalization, such as hydrovoltaic energy generation, sustainable fuels and green chemicals production, and possible indoor environmental improvement. [48][49][50][51] Therefore, further exploration of the interactions between water and functional interfaces and analysis of the strong coupling of multiple physical fields are required. ...

Reference:

Multiscale Heat and Mass Transport Optimization for Solar‐Driven Interfacial Evaporation: Opportunities and Challenges for Industrial Applications
Molecularly Functionalized Biomass Hydrogels for Sustainable Atmospheric Water Harvesting

... The high-entropy configuration of these materials endows them with robust structural stability, conferred by either entropic stabilization or slow diffusion kinetics, thus rendering them viable for use in harsh environments [7,[21][22][23]. HEA catalysts have demonstrated impressive activity and stability across a range of applications, encompassing ammonia synthesis and decomposition [7,[24][25][26][27], water splitting [10,[28][29][30][31][32][33], CO 2 reduction [34][35][36][37][38], and various oxidation [12,[39][40][41][42]. ...

General synthesis of high-entropy single-atom nanocages for electrosynthesis of ammonia from nitrate

... Building upon the integration of advanced hydrogels for water absorption and release, a recent research has combined these properties with nutrient delivery systems. Park et al. introduced a self-irrigation and slow-release fertilizer hydrogel (SISRH) system designed to improve water and nutrient efficiency in agriculture [39]. This hydrogel employs a thermoresponsive interpenetrating network incorporating calcium chloride as both a hygroscopic agent and a nutrient source, enabling it to harvest moisture at night and release water and nutrients during the day ( Figure 4B). ...

Self-Irrigation and Slow-Release Fertilizer Hydrogels for Sustainable Agriculture
  • Citing Article
  • July 2024

ACS Materials Letters

... The results of this study provide a comparison of the performance of three desiccant forms-beaded, powdered, and coated (drop casting)-among four desiccant types, which include zeolite, activated alumina (AA), traditional silica gel, and blue silica gel [21]. Key performance indicators include adsorption capacity, regeneration energy, and kinetics. ...

Chemistries and materials for atmospheric water harvesting
  • Citing Article
  • June 2024

Chemical Society Reviews

... Figure 9(d) shows the device structure of a global smart dimmer using the EC effect. 116 When a voltage is applied, ions from the storage layer are driven through the ion conductor layer toward the EC layer. Afterward, these ions interact with the EC material and cause a redox reaction with a change in the oxidation state of the EC material, resulting in a transmittance change. ...

Sustainable, low-cost, high-contrast electrochromic displays via host–guest interactions

Proceedings of the National Academy of Sciences

... such as light, [1,2] electricity, [3] heat, [4,5] force, [6][7][8] vapor, [9,10] etc. These materials have attracted great attention for their applications in sensing, data storage, and information encryption. ...

Bistable Electrochromic Ionogels via Supramolecular Interactions for Energy‐Efficient Displays

... To circumvent the corrosion impacts of NS, a charge gradient interface strategy has been proposed, in which the gradient-strengthened negative charge toward the Zn surface can induce self-propelled electrostatic forces to boost Zn 2+ diffusion and repel anions. The CGIs are fabricated via diffusion-controlled electrostatic complexation using polysaccharide precursors (Fig. 2a) 14,15 . The chitosan (CS, from natural crab shell) and sodium alginate (SA, from natural seaweed) precursors carry opposite charges due to the respectively protonated -NH 3 + and ionized -COOgroups, as verified by the pH analysis and zeta potential tests (Supplementary Fig. 27 and Fig. 28, and Supplementary Note 3). ...

Sustainable and Rapid Water Purification at the Confined Hydrogel Interface

... Below the LCST, PNIPAM exists in a hydrated, hydrophilic state, where water molecules surround and stabilize the polymer's isopropyl groups, maintaining solubility. Above this temperature, PNIPAM undergoes a reversible phase transition, where increased hydrophobic interactions among isopropyl groups displace water molecules and weaken amide-water hydrogen bonds, leading to polymer-polymer interactions that drive efficient phase separation [37]. These temperature-responsive characteristics of PNIPAM could be strategically adapted to agricultural applications, enabling water release directly into the soil as temperatures shift. ...

Molecularly confined hydration in thermoresponsive hydrogels for efficient atmospheric water harvesting

Proceedings of the National Academy of Sciences

... Despite the emerging controversy over the measurement of evaporation enthalpy, [41] it is undisputed that increasing the intermediate water (IW, also known as freezable bound water) and weakly bonded cluster water in the evaporator to reduce the vaporization enthalpy, and thus accelerate the liquid-gas phase transition. [42] The substrates or photothermal materials with intrinsic hydrophilic groups can form weak hydrogen bonds with water molecules, thus increasing the IW content. Furthermore, hierarchical pore structures and confined nanospace reduce the energy required for evaporation by inducing more water molecule clusters with low vaporization enthalpy. ...

Biomimetically Assembled Sponge‐Like Hydrogels for Efficient Solar Water Purification

... Ideal sorbents are characterized by high water uptake, rapid sorption-desorption kinetics, and operational stability. [12] Material candidates in this field include metal organic frameworks (MOFs), [13,14] salt-based composites, [15][16][17] and hydrogels, [18][19][20][21] each with distinct benefits. MOFs, for instance, facilitate fast water sorptiondesorption, while salt-based composites excel in water uptake. ...

Hygroscopic Microgels-Enabled Rapid Water Extraction from Arid Air