Lei Xie’s research while affiliated with South Central College and other places

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Publications (148)


Effective and selective gold recovery based on synergistic bimetallic-hydroxyl metal–organic frameworks
  • Article

February 2025

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8 Reads

Chemical Engineering Journal

Chaopeng Liu

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Shishuang Zhang

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Preparation and characterization of TMCM‐CdCl3/polymer composite films. a) Schematic comparison of the inhibitory effects of six polymers on the crystallization of TMCM‐CdCl3 and the corresponding bonding interactions. b) Schematic of the co‐dissolution–evaporation method. c) d33 values of different TMCM‐CdCl3/polymer composite films. (n = 10 independent spot d33 measurements on a film. Data are presented as mean ± standard deviation).
Characterization of TMCM‐CdCl3/PEO composite films. a) The d33 values (n = 10 independent spot d33 measurements on a film. Data are presented as mean ± standard deviation.), b) XRD patterns, and c) top‐surface SEM images of films prepared at different TMCM‐CdCl3:PEO mass ratios. d) Cross‐sectional SEM image and EDS maps of a sandwich‐structured film prepared with a TMCM‐CdCl3:PEO mass ratio of 3:2.
Competition mechanism in the TMCM‐CdCl3/PEO composite films. a) Schematic depicting improvement in the crystallization yield of TMCM‐CdCl3 by slightly increasing the amount of one crystal component to compete against PEO for bonding with the other component. b) d33 values of TMCM‐CdCl3/PEO films with one crystal component in excess: the molar ratio of TMCM‐Cl:CdCl2 ranged from 2:1 to 1:2. (n = 10 independent spot d33 measurements on a film. Data are presented as mean ± standard deviation.) c) Comparison of d33 values in this work with those of other previously reported molecular ferroelectric crystal‐based flexible composite films.[19,20,22,56–68]
Mechanical performance of TMCM‐CdCl3/PEO films. a) Stress–strain curves. b) Elastic moduli calculated from the stress–strain curves in a). c) Dynamic mechanical analysis in the frequency sweep mode from 0.1 to 80 Hz at a constant strain of 0.1%. d) Dynamic mechanical analysis in the strain sweep mode from 0.005% to 0.2% strain at a constant frequency of 1 Hz. The films were prepared with mass ratios of TMCM‐CdCl3:PEO ranging from 1:3 to 3:2. The TMCM‐CdCl3/PEO film (denoted as “3:2 (+)”) was prepared with a TMCM‐CdCl3:PEO mass ratio of 3:2 and a TMCM‐Cl:CdCl2 molar ratio of 1.2:1.
Performance of the flexible piezoelectric sensor based on TMCM‐CdCl3/PEO films. a) Schematic diagram and photographs of the sensor. b) Working principle of the sensor. c–e) Electric outputs of the sensors: c) voltage, d) current, and (e) charge under a pulsed 5 N force. f) Variation in the voltage with frequency. g) Durability test. h) Schematic of the sensor placements on the hand. i) Signals from the sensor attached to the index finger joint when bending the finger at different angles. j) Signals from an array of sensors placed on the back of the hand when different fingers tap on the table.

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Bonding Optimization Strategies for Flexibly Preparing Multi‐Component Piezoelectric Crystals
  • Article
  • Publisher preview available

December 2024

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32 Reads

Flexible films with optimal piezoelectric performance and water‐triggered dissolution behavior are fabricated using the co‐dissolution–evaporation method by mixing trimethylchloromethyl ammonium chloride (TMCM‐Cl), CdCl2, and polyethylene oxide (PEO, a water‐soluble polymer). The resultant TMCM trichlorocadmium (TMCM‐CdCl3) crystal/PEO film exhibited the highest piezoelectric coefficient (d33) compared to the films employing other polymers because PEO lacks electrophilic or nucleophilic side‐chain groups and therefore exhibits relatively weaker and fewer bonding interactions with the crystal components. Furthermore, upon slightly increasing the amount of one precursor of TMCM‐CdCl3 during co‐dissolution, this component gained an advantage in the competition against PEO for bonding with the other precursor. This in turn improved the co‐crystallization yield of TMCM‐CdCl3 and further enhanced d33 to ≈71 pC/N, exceeding that of polyvinylidene fluoride (a commercial flexible piezoelectric) and most other molecular ferroelectric crystal‐based flexible films. This study presents an important innovation and progress in the methodology and theory for maintaining a high piezoelectric performance during the preparation of flexible multi‐component piezoelectric crystal films.

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Comparison of different lithium extraction processes: evaporation-precipitation vs EALNF
a, Evaporation-precipitation process: brines are fed into a series of solar evaporitic ponds for sequential precipitation of sodium (Na⁺), potassium (K⁺) and magnesium (Mg²⁺). In the Mg²⁺ pond, a portion of Li⁺ is co-precipitated with Mg²⁺ during Mg²⁺ removal using calcium oxide (CaO), leading to significant Li⁺ loss of ~50% (refs. 24,25). The remaining Li⁺-rich stream is diluted before entering the Li⁺/Mg²⁺ separation unit, which often consists of adsorption and multistage nanofiltration (NF) processes. Concentration units, such as reverse osmosis and/or forced evaporation, follow before the final precipitation stage. b, EALNF process: brine is treated with EDTA⁴⁻ and then directed to a loose nanofiltration unit for direct Li⁺/Mg²⁺ separation. The permeate Li⁺ stream undergoes concentration and purification steps similar to the conventional method, culminating in Li⁺ precipitation where excess Na⁺ and K⁺ are removed by enforced evaporation unit. Concurrently, the retentate stream enters an EDTA⁴⁻ regeneration unit where alkaline agents are added to regenerate EDTA⁴⁻. The regenerated EDTA⁴⁻ stream is recirculated back to the feed brines, enabling continuous operation. Simultaneously, Mg²⁺ ions precipitate from the retentate stream as valuable nanostructured Mg(OH)2 by-products.
Selective binding and filtration of binary-cation brine
a, Schematic representation of the selective binding between Mg²⁺ and EDTA⁴⁻ and their impact on the separation mechanisms within loose nanofiltration membranes. The structures of hydrated Li⁺, hydrated Mg²⁺ and [Mg-EDTA]²⁻ complex were determined by DFT calculations. Mg, yellow; Li, green; O, red; H, grey; C, black; N, blue. b, ¹H-NMR spectra of free EDTA⁴⁻, regenerated EDTA⁴⁻, Mg²⁺/EDTA⁴⁻ mixture and Li⁺/EDTA⁴⁻ mixture. c, Mg²⁺ and [Mg-EDTA]²⁻ rejections by commercial NF membranes. NF-8 membrane was subjected to a 2-h alkaline pretreatment before formal filtration. Three independent experiments were conducted, with individual results represented as dots. d, Effect of salt concentrations on Mg²⁺ rejections at a fixed Li⁺/Mg²⁺ mass ratio of 1:20 and a pressure of 5.0 bar. e, Comparative performance of the XN45 membrane with previously reported NF membranes based on total salt concentration (represented by circle size), Li⁺ permeance and Li⁺/Mg²⁺ separation factor. f, Effects of pressure on Li⁺ flux and permeate Li⁺/Mg²⁺ mass ratio using XN45 membranes. Three independent experiments were conducted, with individual results represented as dots. g, Influence of feed Li⁺/Mg²⁺ mass ratio on (Li⁺/Mg²⁺)Per./(Li⁺/Mg²⁺)Feed using the XN45 membrane. Feed Li⁺ concentration was maintained at 25 mg l⁻¹. Error bars represent s.d.
Source data
Filtration of salt-lake brines
a, Rejection profiles for various ions and b, Li⁺/Mg²⁺ separation factors for Longmu Co Lake brine with and without EDTA⁴⁻ addition. c, Li⁺ flux and Mg²⁺, Li⁺ rejections during a 30-day filtration period of Longmu Co Lake brine with added EDTA⁴⁻. Error bars represent s.d. d–f, Comparative analysis of brine composition (pie charts) and separation performance (spider plots) for (d) Longmu Co Lake brine, (e) diluted Dongtai Lake brine and (f) Dongtai Lake brine. The control group (without EDTA⁴⁻) is represented in grey. Separation performance metrics include Li⁺/Mg²⁺ separation factor (SF), Li⁺ rejection (R-Li⁺), membrane flux (flux, l⁻¹ m⁻² h⁻¹ (LMH)), permeate Li⁺/Mg²⁺ ratio (Per. LMR) and Mg²⁺ rejection (R-Mg²⁺). Unless otherwise specified, all experiments were conducted at a constant pressure of 40 bar using XN45 membranes, selected for their robust performance in high-salinity conditions.
Source data
Comprehensive brine resource utilization and techno-economic analysis
a, R-Mg²⁺ as a function of permeate volume (expressed as P/F ratio) using both pristine and regenerated EDTA⁴⁻ in Longmu Co Lake brine. Experiments were conducted at a constant pressure of 40 bar using XN45 membranes. b, Single-stage Li⁺ recovery and Li⁺/Mg²⁺ ratio in permeate as a function of P/F ratio employing pristine and regenerated EDTA⁴⁻. The green area corresponds to the range of required Li⁺/Mg²⁺ ratio of Li⁺-rich solution in industry. c, XRD patterns of nanostructured Mg(OH)2 by-products during the EDTA⁴⁻ regeneration process. The reference pattern for Mg(OH)2 (PDF# 30-0794) is included for comparison. d–f, SEM images of nanostructured Mg(OH)2 by-products at Mg²⁺ concentrations of (d) ~26.0 g l⁻¹, (e) 1 g l⁻¹ and (f) 0.5 g l⁻¹. These concentrations were achieved by diluting the retentate stream (at a P/F ratio of 0.55) before NaOH addition for EDTA⁴⁻ regeneration. Scale bars, 500 nm. g, Material flow diagram illustrating the EALNF process and associated costs for producing 1 tonne of Li2CO3. h, Comparative cost, income and profit analysis of EALNF and conventional evaporation-precipitation processes for producing 1 tonne of Li2CO3.
Source data
Sustainable lithium extraction and magnesium hydroxide co-production from salt-lake brines

October 2024

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345 Reads

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3 Citations

Nature Sustainability

In recent years, the demand for lithium (Li) has been on the rise as Li-ion batteries are playing an increasingly important role in powering the global transition to a low-carbon society. In contrast to the predominant production of lithium from hard rock, lithium extraction from brine sources has proven more economical and sustainable. However, substantial challenges remain, including the low efficiency of the extraction process, especially for brines of high salinity, complex composition and poor selectivity against magnesium, the major competing species. Here we show a loose nanofiltration process involving ethylenediaminetetraacetic acid (EDTA) for direct and efficient Li⁺ extraction as well as effective Mg²⁺ utilization from salt-lake brines. Taking advantage of selective binding between EDTA⁴⁻ and Mg²⁺, our process achieves ultrahigh Mg²⁺ rejection of 99.85%, ultrafast Li⁺ flux of ~4.34 mol m⁻² h⁻¹ and unprecedented Li⁺/Mg²⁺ separation factor (~679) under industrial conditions (127.06 g l⁻¹). More importantly, the Li⁺ recovery rate reaches 89.90% through a two-stage filtration process, while Mg²⁺ waste is converted to nanostructured Mg(OH)2 and 98.87% of EDTA⁴⁻ can be regenerated. Our scalable process minimizes environmental impact while maximizing resource utilization, thereby catalysing the shift toward a more sustainable future.




Molecular Interaction Mechanisms Between Lubricant-Infused Slippery Surfaces and Mussel-Inspired Polydopamine Adhesive and DOPA Moiety

July 2024

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20 Reads

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2 Citations

Macromolecular Rapid Communications

Lubricant‐infused slippery surfaces have recently emerged as promising antifouling coatings, showing potential against proteins, cells, and marine mussels. However, a comprehensive understanding of the molecular binding behaviors and interaction strength of foulants to these surfaces is lacking. In this work, mussel‐inspired chemistry based on catechol‐containing chemicals including 3,4‐dihydroxyphenylalanine (DOPA) and polydopamine (PDA) is employed to investigate the antifouling performance and repellence mechanisms of fluorinated‐based slippery surface, and the correlated interaction mechanisms are probed using atomic force microscopy (AFM). Intermolecular force measurements and deposition experiments between PDA and the surface reveal the ability of lubricant film to inhibit the contact of PDA particles with the substrate. Moreover, the binding mechanisms and bond dissociation energy between a single DOPA moiety and the lubricant‐infused slippery surface are quantitatively investigated employing single‐molecule force spectroscopy based on AFM (SM‐AFM), which reveal that the infused lubricant layer can remarkably influence the dissociation forces and weaken the binding strength between DOPA and underneath per‐fluorinated monolayer surface. This work provides new nanomechanical insights into the fundamental antifouling mechanisms of the lubricant‐infused slippery surfaces against mussel‐derived adhesive chemicals, with important implications for the design of lubricant‐infused materials and other novel antifouling platforms for various bioengineering and engineering applications.




Probing the surface forces between air bubbles and bitumen via direct force Measurements: Effects of aqueous chemistry

February 2024

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99 Reads

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1 Citation

Fuel

A R T I C L E I N F O Keywords: bitumen oil sands bitumen flotation bubbles surface interactions A B S T R A C T The surface interactions of air bubbles and other components (e.g., particles, oil droplets) significantly influence the operation efficiency of a variety of engineering processes such as oily water treatment, bitumen extraction and flotation. Herein, the surface interactions of air bubbles with two types of Athabasca bitumen samples in aqueous solutions of varying pH, salinity, type of cations and in the presence of surfactants have been systematically characterized using a bubble probe atomic force microscope (AFM) technique. AFM imaging has revealed that exposure to high concentrations of NaCl and CaCl 2 solutions or alkaline environments causes roughening of the bitumen surfaces. The results of surface force measurements demonstrate that the interaction and attachment behaviors between bubbles and bitumen are significantly affected by ionic strength, solution pH, and the presence of surfactants. The experimental force measurement results could be accurately described by a theoretical model that incorporates Reynolds lubrication theory and augmented Young-Laplace equation, with the inclusion of disjoining pressure. In low-salinity conditions, the bubble-bitumen interaction is dominated by electric double layer (EDL) repulsion, which prevents surface attachment. This effect is more pronounced at elevated pH conditions. In high-salinity solutions, however, the EDL interactions are significantly reduced, and the hydrophobic interaction becomes the dominant factor, overcoming the van der Waals repulsion and leading to the attachment of bubbles to bitumen surfaces. Raising aqueous pH weakens the bubble-bitumen hydrophobic interaction, whereas the introduction of calcium ions strengthens this interaction, resulting in enhanced surface attachment. Interestingly, even in high-salinity conditions, the presence of a small number of surfactants can inhibit bubble-bitumen contact, mainly caused by reduced hydrophobic attraction and increased steric repulsion. This work provides valuable nanoscale insights into how bubbles and bitumen interact in intricate aqueous environments, and the results show practical implications for controlling similar interfacial phenomena in various engineering processes.


Citations (61)


... Nevertheless, the physicochemical similarities between Li + and Mg 2+ remain a challenge to their efficient separation. Now, writing in Nature Sustainability, Yong et al. present a loose nanofiltration method that uses ethylenediaminetetraacetic acid (EDTA) for efficient Li + extraction from salt-lake brines while enabling Mg 2+ utilization 7 . ...

Reference:

Lithium recovery from brines
Sustainable lithium extraction and magnesium hydroxide co-production from salt-lake brines

Nature Sustainability

... Moreover, organic compounds such as humic and fulvic acids can adsorb onto the NCC surface, altering its surface properties and reducing its adsorption capacity for Pb and As. These acids also affect the speciation of Pb and As in solution by modifying the pH of the medium, thereby indirectly affecting their adsorption [101,102]. ...

Nanoscale Insights into the Interaction Mechanism Underlying the Adsorption and Retention of Heavy Metal Ions by Humic Acid
  • Citing Article
  • January 2024

Environmental Science and Technology

... However, it is recommended to use adsorption approaches to reduce the harmful effects of the resulting chemical intermediates during the oxidation and catalytic decomposition processes (Neolaka et al., 2023a;Wu et al., 2023). Numerous studies indicate that adsorption using new materials is an affordable, effective, safe, readily available, and recoverable method for the decontamination of diverse water contaminants Wang et al., 2024). The selection of a successful adsorbing material is affected by various factors, involving production expenses, production processes, precursor availability, adsorption efficiency, recyclability, uptake capacity, biodegradability, uptake specificity, safety, durability, and reactivity (Fan et al., 2024;Khattari et al., 2024). ...

Facet-dependent Adsorption of Heavy Metal Ions on Janus Clay Nanosheets
  • Citing Article
  • September 2023

Journal of Hazardous Materials

... To explain how the bonding interactions vary depending on the type of polymer, we conducted quantitative comparison of adhesion energies between different polymer and TMCM-CdCl 3 components using atomic force microscopy ( Figure S5, Supporting Information), [48,49] and by Density functional theory (DFT) calculations of the integrated crystal orbital Hamilton population (ICOHP) values of halogen and hydrogen bonds formed between polymers and TMCM-CdCl 3 . [50][51][52][53] The comparison results of adhesion energies (Figures S6-S8, Supporting Information), and calculated |ICOHP| values ( Figure S9, Table S1, Supporting Information) are consistent with the comparison of bonding interactions described above. ...

Deciphering the specific interaction of humic acid with divalent cations at the nanoscale
  • Citing Article
  • June 2023

Chemical Engineering Journal

... The factors of PT toxicity for plants are (1) high acidity (pH < 4.5) and (2) chemical imbalance, viz., an extremely high content of metals and low contents of calcium and magnesium. In turn, the mineral and chemical compositions of serpentine products justify the expediency of their use to improve the PT properties, since serpentines are capable of reacting with acid solutions in the reaction of neutralization, absorbing metals, and increasing the calcium and magnesium contents in the soil solution [4,5]. However, the method of remediation by covering polluted soil with mineral material does not make it possible to use fully the positive potential of favorable properties of peat soil for ecosystems, such as a high water content, the presence of organic matter and microbial biomass reserves, and the associated nutrient reserves, primarily nitrogen. ...

Cd(II) adsorption on earth-abundant serpentine in aqueous environment: Role of interfacial ion specificity
  • Citing Article
  • May 2023

Environmental Pollution

... Therefore, the hydrophobic modification of polar adsorbents could be advantageous for BPA adsorption. Similar to the general tendency of hydrophobic organic materials, they adsorb extensively on hydrophobic mineral surfaces due to attractive hydrophobic interactions in aqueous solution [32]. The hydrophobic interactions often manifest themself such as micelle formation, protein folding, hydrophobic contaminant adsorption at the air-water interface, their quantitative understanding has been a topic of considerable interest for decades but remains elusive [33]. ...

Nanomechanical Insights into Hydrophobic Interactions of Mineral Surfaces in Interfacial Adsorption, Aggregation and Flotation Processes
  • Citing Article
  • November 2022

Chemical Engineering Journal

... To address these issues, many techniques have been used, including pretraining (Pino et al., 2020;Alinejad and Sarkar, 2020;Dong et al., 2021;, multi-task learning (Tang et al., 2021;Ye et al., 2021b;Vydana et al., 2021), data augmentation Mi et al., 2022), metalearning (Indurthi et al., 2020), and cross-modal alignment (Han et al., 2021;Fang et al., 2022). While most research chose to migrate the translation ability from MT to ST by designing exquisite model architectures or training procedures, few studies have investigated the correlation between speech characteristics and translation performance. ...

Improving data augmentation for low resource speech-to-text translation with diverse paraphrasing
  • Citing Article
  • February 2022

Neural Networks

... As an automated machine learning technique [15], [22], NAS has been widely used for many research domains [23] and made significant progress since first proposed in [24]. Existing NAS approaches have been used for various domains to search the best architectures of various prevailing DNNs, including CNNs for computer vision (CV) tasks [25], RNNs for natural language processing (NLP) [17] and speechrelated [18] tasks, GNNs for non-Euclidean data tasks [26], and Transformers for CV [27], NLP [28], and speechrelated [29] tasks. ...

Efficient Gradient-Based Neural Architecture Search For End-to-End ASR
  • Citing Conference Paper
  • October 2021

... Fig. 3 provides an illustration of the working principles of the AFM [40]. Various AFM probes have been used for imaging and force measurements, including: a sharp tip, a colloid probe made by gluing a colloidal particle to a tipless cantilever, and bubble and drop probes made by attaching a gas bubble or liquid droplet to a tipless cantilever, as shown in Fig. 3 [16][17][18][41][42][43][44][45][46][47][48][49]. The colloid probe enables the surface force measurements of various particle materials (e.g., minerals, polymers, and cells). ...

Probing Hydrophobic Interactions between Polymer Surfaces and Air Bubbles or Oil Droplets: Effects of Molecular Weight and Surfactants
  • Citing Article
  • November 2021

Langmuir

... This imperfect surface O coordination state facilitates the covalent reactions between these minerals and organic functional groups or metal(loid)s. Additionally, these minerals grow and dissolve readily, forming particles in diverse shapes depending on the chemical composition of the nascent solution (Xie et al., 2021). The relatively high interfacial energy of these minerals enables the coexistence of multiple Fe (hydr)oxides, as differences in surface and bulk energies cause reversals in the order of thermodynamic stability as a function of particle size and aqueous chemistry (Guo & Barnard, 2013;Navrotsky et al., 2008). ...

Surface interaction mechanisms in mineral flotation: Fundamentals, measurements, and perspectives
  • Citing Article
  • July 2021

Advances in Colloid and Interface Science