Huaping Zhao’s research while affiliated with Technische Universität Ilmenau and other places

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Publications (152)


Schematic diagram of the synthesis process of CSS‐C0, CSS‐C1, and CSS‐C2, respectively.
a) XRD patterns of CSS‐C0, CSS‐C1, and CSS‐C2, respectively. b) Raman spectra and c) FTIR spectra of CSS‐C1 and CSS‐C2, respectively.
a) SEM image, b) TEM image, c) HRTEM image with corresponding lattice spacing and SAED pattern, and d) element mapping images of CSS‐C1, respectively.
High‐ resolution XPS spectrum of a) Co 2p, b) Sn 3d, and c) S 2p for CSS‐C0, CSS‐C1, and CSS‐C2, respectively.
a) CV curves of CSS‐C1 at 0.1 mV s⁻¹ within voltage ranges of 0.01–3 V. b) Ex situ XRD patterns corresponding to different voltages. c) Charge/discharge profiles of CSS‐C1 at 0.1 A g⁻¹ within voltage ranges of 0.01‐3 V. d) Rate performance CSS‐C0, CSS‐C1, and CSS‐C2, respectively. Cycling performance at e) 0.5 A g⁻¹ and f) 10 A g⁻¹ of CSS‐C0, CSS‐C1, and CSS‐C2, respectively. g) XRD patterns of CSS‐C1 anodes after different cycles.

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Enhanced Stability of Sodium‐Ion Batteries by Controlling the Synthesis Process of Binary Metal Sulfides
  • Article
  • Full-text available

March 2025

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19 Reads

Wenbo Qiu

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Zidong Wang

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Huaping Zhao

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[...]

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Binary metal sulfides hold significant promise as anode materials for advanced sodium‐ion batteries (SIBs), but their application is often limited by rapid capacity degradation and slow reaction kinetics. While carbon composites are frequently used to address these issues, the influence of the sequence of carbonization and sulfidation on anode performance has been largely overlooked. To bridge this gap, Co‐Sn sulfides are synthesized through various processes to examine the impact of synthesis methods on material properties. Among these, the one‐step synthesized CSS‐C1 exhibits enhanced sodium‐ion kinetics and excellent stability. It delivers a capacity of 220.4 mAh g⁻¹ at an ultra‐high current density of 20 A g⁻¹ and maintained 389 mAh g⁻¹ over 2300 cycles at 10 A g⁻¹. When assembled into full‐cell devices (CSS‐C1||Na3V2(PO4)3), it demonstrates stable capacity retention for over 900 cycles, establishing it as a highly stable and efficient anode material for SIBs.

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The structural feature comparison of single‐atom catalyst, dual‐atom catalyst and atomic symbiotic‐catalyst.
Synthesis and structural characterization of the MnN4/Cd ASC. (a) Schematic illustration of the MG precursor strategy to synthesize the MnN4/Cd ASC. (b) SEM, (c) TEM, (d) HRTEM and SAED pattern of MnN4/Cd ASC. (e) HAADF‐STEM image of MnN4/Cd ASC. (f) Element maps of MnN4/Cd ASC, Mn (purple), C (blue), N (red), respectively. (g) AC‐HAADF‐STEM image of MnN4/Cd ASC.
Microenvironment characterization of the MnNx/Cd ASCs. (a) Mn K‐edge XANES spectra. (b) Mn K‐edge FT‐EXAFS spectra. (c) WT‐EXAFS of MnN4/Cd ASC. (d) EXAFS R space fitting curves of MnN5/Cd ASC. (e) EXAFS R space fitting curves of MnN4/Cd ASC. (f) EXAFS R space fitting curves of MnN3/Cd ASC. (g) N 1s and (h) C 1s XPS spectra of the MnNx/Cd ASCs. (i) Raman spectra of the NC and MnNx/Cd ASCs.
Electrochemical and ZAB performances of MnNx/Cd ASCs. (a) ORR polarization curves of MnNx/Cd and reference catalysts in 0.1 M KOH. (b) Comparison of mass activities and E1/2 of MnNx/Cd and reference catalysts. (c) ORR polarization curves of initial MnN4/Cd and after 5000, 10000 and 15000 potential cycles. (d) The comparison of GCD curves at 1 A g⁻¹ for the MnNx/Cd and NC samples measured in three‐electrode configuration using 6 M KOH as electrolyte. (e) Plots of specific capacitance versus current density for the MnNx/Cd and NC samples. (f) Comparison of E1/2 for MnN4/Cd and 20 % Pt/C in KOH electrolytes with different concentrations. (g) Open circuit voltage plots of flexible solid‐state ZABs based on MnN4/Cd and Pt/C as air cathodes with different concentrations (6, 4, 2 M) of KOH electrolyte at −40 °C. (h) Power density curves of the flexible solid‐state ZABs at −40 °C. (i) Comprehensive comparison of the ZAB performances based on MnN4/Cd and other reported state‐of‐the‐art catalysts. References are provided in Table S3 (highlighted in blue).
DFT calculation results showing the ORR mechanism with K⁺ cation. (a) Atomic configurations of MnN4/Cd ASC with sp³ carbon at different sites. Mn and N atoms are marked by pink and blue, respectively. The sp³ carbon is marked by black. (b) Adsorption energies of K⁺ cation on different sites of MnN4/Cd ASC according to (a). (c) Atomic configuration with the lowest adsorption energy according to (b). K⁺ cations are marked by purple. (d) PDOS on different carbon atoms. (e) PDOS on Mn ion in different systems, (f) Free energy diagrams of ORR on MnN4/sp²‐C (black), MnN4/sp³‐C when K⁺ is at site1 (red), and MnN4/sp³‐C when K⁺ is at site3 (blue). Left panel is the atomic configurations of intermediates during the pathway MnN4/K+sp³‐C site3 according to the right panel.
Atomic Symbiotic‐Catalyst for Low‐Temperature Zinc‐Air Battery

March 2025

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60 Reads

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1 Citation

Atomic‐level designed electrocatalysts, including single‐/dual‐atom catalysts, have attracted extensive interests due to their maximized atom utilization efficiency and increased activity. Herein, a new electrocatalyst system termed as “atomic symbiotic‐catalyst”, that marries the advantages of typical single‐/dual‐atom catalysts while addressing their respective weaknesses, was proposed. In atomic symbiotic‐catalyst, single‐atom MNx and local carbon defects formed under a specific thermodynamic condition, act synergistically to achieve high electrocatalytic activity and battery efficiency. This symbiotic‐catalyst shows greater structural precision and preparation accessibility than those of dual‐atom catalysts owing to its reduced complexity in chemical space. Meanwhile, it outperforms the intrinsic activities of conventional single‐atom catalysts due to multi‐active‐sites synergistic effect. As a proof‐of‐concept study, an atomic symbiotic‐catalyst comprising single‐atom MnN4 moieties and abundant sp³‐hybridized carbon defects was constructed for low‐temperature zinc‐air battery, which exhibited a high peak power density of 76 mW cm⁻² with long‐term stability at −40 °C, representing a top‐level performance of such batteries.


Atomic Symbiotic‐Catalyst for Low‐Temperature Zinc‐Air Battery

March 2025

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12 Reads

Angewandte Chemie

Atomic‐level designed electrocatalysts, including single‐/dual‐atom catalysts, have attracted extensive interests due to their maximized atom utilization efficiency and increased activity. Herein, a new electrocatalyst system termed as “atomic symbiotic‐catalyst”, that marries the advantages of typical single‐/dual‐atom catalysts while addressing their respective weaknesses, was proposed. In atomic symbiotic‐catalyst, single‐atom MN x and local carbon defects formed under a specific thermodynamic condition, act synergistically to achieve high electrocatalytic activity and battery efficiency. This symbiotic‐catalyst shows greater structural precision and preparation accessibility than those of dual‐atom catalysts owing to its reduced complexity in chemical space. Meanwhile, it outperforms the intrinsic activities of conventional single‐atom catalysts due to multi‐active‐sites synergistic effect. As a proof‐of‐concept study, an atomic symbiotic‐catalyst comprising single‐atom MnN 4 moieties and abundant sp ³ ‐hybridized carbon defects was constructed for low‐temperature zinc‐air battery, which exhibited a high peak power density of 76 mW cm ⁻² with long‐term stability at −40 °C, representing a top‐level performance of such batteries.


Facilitating Sodium‐Ion Diffusion in Fe‐Doped Co3O4 for High‐Rate Performance

February 2025

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37 Reads

Due to its high theoretical capacity, cobalt oxide (Co3O4) has attracted attention to sodium‐ion battery (SIB) anodes. However, its low conductivity and poor rate performance have limited its practical application. This work proposes a co‐precipitation doping strategy to synthesize iron‐doped Co3O4 nanoparticles (FexCo3‐xO4 NPs). Both experimental and theoretical results confirm that iron (Fe) doping at octahedral sites within spinel structures is a critical factor in enhancing rate performance. The decreased bandgap and enlarged ion transport spacing originate in Fe doping. This effectively facilitates the electron and Na‐ion (Na⁺) transport during discharge/charge processes, delivering an impressive rate capability of 402.9 mAh g⁻¹ at 3 A g⁻¹. The FexCo3‐xO4 NPs demonstrate remarkable cycling stability. They maintain a high specific capacity of 786.2 mAh g⁻¹ even after 500 cycles at 0.5 A g⁻¹, with no noticeable capacity fading. When assembled into a Na‐ion full cell, a remarkable discharge capacity of 105 mAh g⁻¹ with stable cycling performance is attained. This work provides valuable insights into the functional design of high‐rate electrodes, offering a promising approach to addressing the critical challenges faced by sodium anodes.


Solubility Challenges and Strategies for Organic Sodium‐Ion Batteries: Status and Perspectives

February 2025

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20 Reads

Organic sodium‐ion batteries (OSIBs) possessing excellent characteristics of low price, abundant sources, and eco‐compatibility have gained numerous attentions in the recent decade. However, solubility is one of the main severe limitations of the application of OSIBs, especially for small organic molecules. The dissolution of molecules into electrolytes can cause the loss of active materials, the pulverization of electrodes, and even short circuits in batteries, as active materials may shuttle through separators, thus leading to poor cycling stability for sodium‐ion batteries. Thus, there is an urgent need to develop insoluble organic molecules for OSIBs. The advanced development of OSIBs over the past decades is overviewed, and the primary challenges faced by long‐cycling OSIBs in terms of solubility are systematically analyzed. Focusing on the three core components of the battery system electrodes, separators, and electrolytes, targeted optimization strategies are proposed to mitigate solubility issues and enhance battery performance. In addition, the prospects of OSIBs toward long‐cycle stability and practical application are explored.


Catalyzed carbon-based materials for CO 2 -battery utilization

January 2025

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60 Reads

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1 Citation

Increasing atmospheric CO2 levels and global carbon neutrality goals have driven interest in technologies that both mitigate CO2 emissions and provide sustainable energy storage solutions. Metal-carbon dioxide (M-CO2) batteries offer significant promise due to their high energy density and potential to utilize atmospheric CO2. A key challenge in advancing M-CO2 batteries lies in optimizing CO2-breathing cathodes, which are essential for CO2 adsorption, diffusion, and conversion. Carbon-based cathodes play a critical role in facilitating CO2 redox for M-CO2 batteries, owing to their cost-effectiveness, high conductivity, tunable microstructure, and porosity. However, there is a lack of current systematic understanding of the relationship between the structure, composition, and catalytic properties of carbon-based cathodes, as well as their impact on the overall efficiency, stability, and durability of M-CO2 batteries. In this review, we will give an insightful review and analysis of recent advances in various carbon-based materials, including commercial carbons, single-atom catalysts, transition metal/carbon composites, metal-organic frameworks, etc. , focusing on their structure-function-property relationships. A comprehensive understanding of the pivotal role played by carbon-based materials and their optimization strategies in M-CO2 batteries will be provided. Moreover, future perspectives and research suggestions for carbon-based materials are presented to advance the development and innovation of M-CO2 batteries.





Multiscale Defective Interfaces for Realizing Na‐CO2 Batteries With Ultralong Lifespan

October 2024

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69 Reads

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3 Citations

Despite their favorable high energy density and potential for CO2 recycling, Na‐CO2 batteries have been held back by limitations in cycling capability, stemming from the sluggish CO2 reduction/evolution reaction (CO2RR/CO2ER) kinetics at CO2 cathode and unmanageable deposition/stripping of metallic Na at the anode upon cycling. Herein, a “two‐in‐one” electrode with multiscale defective FeCu interfaces (CP@FeCu) is presented, which is capable of improving the CO2RR/CO2ER kinetics of CO2‐breathing cathode, while modulating sodium deposition behavior. Experimental and theoretical investigations reveal multiscale defective FeCu interfaces are responsible for the enhancement of sodiophilicity and catalytic properties. The defect and valence oscillation effects originate in multiscale defective FeCu interfaces, effectively facilitating the adsorption of reactants and decomposition of Na2CO3 during CO2RR/CO2ER processes, along with exceptional cycling stability of 2400 cycles (4800 h) at 5 µA cm⁻². Meanwhile, the CP@FeCu with sodium affinity creates a uniform electric field and robust adsorption for Na, making initial nucleation sites more conducive to Na deposition and achieving dendrite‐resistant and durable anodes. This work offers a scientific insight into the functionalization design of “two‐in‐one” electrodes, which is essential for a unified solution to the challenges in sodium anodes and CO2 cathodes.


Citations (75)


... In contrast, the spectrum of LLTO/ZIF-8@IL/PEO shows clear cross-peaks at the dashed box positions (Fig. 4(k)), suggesting a significant enhancement in the Li + exchange rate between LLTO and PEO. A more vivid explanation is that Li + can "swim" through the "canyon" in a solvated form (Fig. 4(l)), facilitating their smooth transport from the PEO matrix to LLTO phase [39][40][41][42][43][44][45]. ...

Reference:

Enhanced Li + transport across the organic-inorganic interface in composite solid electrolytes via a confined solvation strategy
Atomic Symbiotic‐Catalyst for Low‐Temperature Zinc‐Air Battery

... Very recently, our group put forward a multiscale defective interface concept via atomic misfit-driven reconfiguration to design a CO 2 cathode (Figure 9a). [193] It is pleasing to note that this self-supporting CO 2 cathode regulates the adsorption/decomposition of intermediates during CO 2 RR/CO 2 ER and ensures exceptional operation of the Na-CO 2 battery for 2400 cycles (4800 h). ...

Multiscale Defective Interfaces for Realizing Na‐CO2 Batteries With Ultralong Lifespan

... Biomass-derived carbon materials refer to the carbon material prepared from natural biomass sources such as wood [15], straw [16], bamboo [17], etc. When compared to traditional carbon sources, carbon materials derived from biomass offer the benefits of being both renewable and cheap [18][19][20]. ...

Boosting the Energy Density of Bowl‐Like MnO2@Carbon Through Lithium‐Intercalation in a High‐Voltage Asymmetric Supercapacitor with “Water‐In‐Salt” Electrolyte

... Although a MoS 2 /r-GO/CNT fiber with a H 2 SO 4 /PVA electrolyte showed a comparable energy density (26.4 Wh kg −1 ), it could only operate at a much lower power density (4,000 W kg −1 ). This exceptional overall performance stems from the synergistic combination of the enhanced ionic conductivity (73.5 mS cm −1 ) achieved through optimized HT concentration and the excellent interfacial compatibility between the VG@CNTF electrode and HT_RPE [55][56][57][58]. ...

Insights into Nano- and Micro-Structured Scaffolds for Advanced Electrochemical Energy Storage

Nano-Micro Letters

... Recently, with the development of synthesis techniques and precise adjustment of surface parameters, the surface morphology and mechanical properties of TiO2-based nanomaterials have been changed. Examples include the fabrication of nanodots [16], nanopillar [17], and nanoneedles. Salatto et al. synthesized the vertically oriented polystyrene-block-poly(methyl methacrylate) cylindrical nanostructure and coated it on TiO2 nanopillars. ...

Unique gap-related SERS behaviors of p-aminothiophenol molecules absorbed on TiO2 surface in periodic TiO2/Ni nanopillar arrays

... The resulting diffraction pattern shows that the increase in the substitution of Ni and Ti ions (x = 0; 0.03; 0.05; 0.1) causes a change in intensity and a shift in peak position without changing the XRD pattern ( Figure 1). He et al. (2024) stated that this 2 shift indicated that there had been a replacement of cations in the compound lattice. So, in this study, the intensity and peak ...

Effect of Partial Cation Replacement on Anode Performance of Sodium-Ion Batteries

... This enlarged spacing allows for better insertion of ions compared to VS 2 , where the lower sulfur content results in tighter interlayer distances. The easier accommodation of ions leads to more effective ion insertion, enhancing the energy storage capacity [16][17][18]. Sulfur-doped porous carbons can achieve high specific surface areas (670-2210 m 2 /g) and pore volumes (0.31-1.26 cm 3 /g) through controlled activation processes [19]. Adding sulfides increases porosity and alters the micromorphology, with the number of fine particles on the surface increasing significantly [20]. ...

Research Progress on Vanadium Sulfide Anode Materials for Sodium and Potassium‐Ion Batteries

... In addition, two satellite peaks were observed at 861.5 eV and 897.6 eV [25,26]. Figure 3c shows the peaks of Co 2p: the peaks at 783.1 eV, 798.9 eV and 780.4 eV, 796.2 eV correspond to the valence states of Co 2+ and Co 3+ of Co 2p, respectively, as well as two satellite peaks (786.1 eV, 802.4 eV) in their vicinity [27]. ...

Rational Design of a Hierarchical Candied-Haws-like NiCo 2 O 4 @Ni,Co-(HCO 3 ) 2 Heterostructure for the Electrochemical Performance Enhancement of Supercapacitors
  • Citing Article
  • September 2023

ACS Applied Energy Materials

... As the discharge continues, multiple nanosheets stack together, which corresponds to the ORR proceeding on the Pt electrode (Fig. 1d). The thin nanosheets keep growing and propagating along the horizontal direction (Fig. 1e, f), which possess a large contact area with the substrate and may contribute to a reduced Gibbs free energy during the following decomposition reaction 27,28 . No sediments can be found in the experimental conditions under Ar ( Supplementary Fig. S6). ...

Gel Adsorbed Redox Mediators Tempo as Integrated Solid‐State Cathode for Ultra‐Long Life Quasi‐Solid‐State Na–Air Battery

... With the commercialization of sodium-ion batteries (SIBs), as more sustainable and cost-effective alternative solutions for energy storage, the understanding of the SEI formation, its dynamic behavior and its composition is crucial. [13][14][15] Hard carbon (HC) is one of the most widely used anode materials for SIBs due to its excellent storage capacity for sodium ions, the low operating voltage, its high reversible specific capacity, high conductivity and the low cost. [16][17][18] A previous study has shown significantly different lifetimes for cells using HC, which is likely attributed to differences in the electrolyte used, the mass loading of the electrode with the active material, the C-rates, or other experimental conditions. ...

Research progress of solid electrolyte interphase for sodium metal anodes
  • Citing Article
  • September 2023

Chemical Engineering Journal