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Optimizing the ORR performance of PtMnM ternary intermetallics by tuning the surface strain

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Science China chemistry 2025年第2期68卷 536-542页

作者： Min Song Guanyu Luo Qian Zhang Hanyu Hu Deli Wang key laboratory of Material chemistry for energy conversion and storage Ministry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and Technology(HUST)Wuhan 430074China

Identifying the descriptors that control catalytic performance is key to design catalysts with high activity and *** indirect descriptors related to catalytic activity,modulating the Pt–Pt interatomic distance and d-band center can effectively enhance the ORR *** is well recognized that the Pt–Pt interatomic distance is strongly correlated with the surface ***,PtMnM/C ternary intermetallics are constructed through partially replacing Mn in PtMn/C binary intermetallics with the other transition metal(M=Fe,Co,Ni,and Cu).The 3d-transition metal doping induces surface strain,and the ORR performance of PtMnM/C exhibits volcano relationship relative to both the Pt–Pt interatomic distance and d-band *** PtMnCo/C with optimum strain exhibits the highest mass activity(1.06 A mgPt^(−1))at 0.9 V,which is 2.6 and 4.6 times higher than that of PtMn/C and commercial Pt/C catalysts,*** addition,PtMnCo/C shows good durability with only 10 mV half-wave potential decay after 50,000 potential cycles.

关键词： oxygen reduction reaction electrocatalysts ternary intermetallics surface strain electronic structure

Building Li-S batteries with enhanced temperature adaptability via a redox-active COF-based barrier-trapping electrocatalyst

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Journal of energy chemistry 2025年第2期101卷 702-712页

作者： Jie Xu Acheng Zhu Zhangyu Zheng Yiming Qi Yuwen Cheng Yongjie Cao Bo Peng Lianbo Ma Yonggang Wang School of materials Science and Engineering Key Laboratory of Efficient Conversion and Solid-state Storage of Hydrogen & Electricity of Anhui Province Key Laboratory of Green Fabrication and Surface Technology of Advanced Metal Materials of Ministry of Education Anhui University of Technology Department of chemistry and Shanghai key laboratory of Molecular Catalysis and Innovative materials Institute of New Energy iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Fudan University

Covalent organic frameworks（COFs） are promising materials for mitigating polysulfide shuttling in lithium-sulfur（Li-S） batteries,but enhancing their ability to convert polysulfides across a wide temperature range remains a challenge,Herein,we introduce a redox-active COF（RaCOF） that functions as both a physical barrier and a kinetic enhancer to improve the temperature adaptability of Li-S batteries,The RaCOF constructed from redox-active anthraquinone units accelerates polysulfide conversion kinetics through reversible C=O/C-OLi transformations within a voltage range of 1,7 to 2.8 V（***+/Li）,optimizing sulfur redox reactions in ether-based *** conventional COFs,RaCOF provides bidentate trapping of polysulfides,increasing binding energy and facilitating more effective polysulfide ***-situ XRD and ToF-SIMS analyses confirm that RaCOF enhances polysulfide adsorption and promotes the transformation of lithium sulfide（Li2S）,leading to better sulfur cathode ***,RaCOF-modified Li-S batteries demonstrate low self-discharge（4.0% decay over a 7-day rest）,excellent wide-temperature performance（stable from-10 to+60℃）,and high-rate cycling stability（94% capacity retention over 500 cycles at 5.0 C）.This work offers valuable insights for designing COF structures aimed at achieving temperature-adaptive performance in rechargeable batteries.

关键词： Covalent organic framework Lithium-sulfur batteries Redox-active property Wide-temperature adaptability

Improving structure stability of single-crystalline Ni-rich cathode at high voltage by element gradient doping and interfacial modifcation

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Journal of energy chemistry 2025年第2期101卷 630-640页

作者： Ruijuan Wang Yixu Zhang Zhi Li Lei Wu Jiarui Chen Xiaolin Liu Hui Hu Hao Ding Shuang Cao Qiliang Wei Xianyou Wang National Base for International Science & Technology Cooperation of New energy Equipment Energy Storage Materials and Devices National Local Joint Engineering Laboratory for Key Materials of New Energy Storage Battery Hunan Province Key Laboratory of Electrochemical Energy Storage & Conversion School of Chemistry Xiangtan University Institute of Micro/Nano materials and Devices Ningbo University of Technology

Single-crystalline Ni-rich cathodes can provide high energy density and capacity retention rates for lithium-ion batteries（LIBs）.However,single-crystalline Ni-rich cathodes experience severe transition metal dissolution,irreversible phase transitions,and reduced structural stability during prolonged cycling at high voltage,which will significantly hinder their practical ***,a Li4TeO5surface coating along with bulk Te-gradient doping strategy is proposed and developed to solve these issues for single-crystalline Ni-rich LiNi0.90Co0.05Mn0.05O2cathode（LTeO-1.0）.It has been found that the bulk Te6+gradient doping can lead to the formation of robust Te-O bonds that effectively inhibit H2-H3 phase transformations and reinforce the lattice framework,and the in-situ Li4TeO5coating layer can act as a protective layer that suppresses the parasitic reactions and grain ***,the modified material exhibits a higher Young's modulus,which will be conducive to maintaining significant structural and electrochemical stability under high-voltage conditions,Especially,the LTeO-1.0 electrode shows the improved Li+diffusion kinetics and thermodynamic stability as well as high capacity retention of 95.83%and 82.12% after 200 cycles at the cut-off voltage of 4.3 and 4,5 ***,the efficacious dualmodification strategy will definitely contribute to enhancing the structural and electrochemical stability of single-crystalline Ni-rich cathodes and developing their application in LIBs.

关键词： High cut-off voltage Li4TeO5 coating layer Material fragmentation Single-crystalline Ni-rich cathode Te6+ doping

Selenate-based heterojunction with cobalt-nickel paired site for electrocatalytic oxidation of 5-hydroxymethylfurfural coupling water splitting to produce hydrogen

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Journal of energy chemistry 2025年第2期101卷 156-162页

作者： Zhengru Yang Jia Hui Wangxi Fan Pengcheng Liu Chunyong Zhang Shuang Dong Zhou Yang Department of chemistry and Chemical Engineering & Jiangsu Key Laboratory of Clean Energy Storage and Conversion Jiangsu University of Technology Engineering Technology and materials Research Center China Academy of Transportation Sciences School of Chemical Engineering and materials Changzhou Institute of Technology

It is very appealing that 5-hydroxymethylfurfural（HMF） is electrocatalytical oxidized as 2,5-furandicarboxylic acid（FDCA） linking to non-classical cathodic hydrogen（H2） ***,the electrocatalysts for electrocatalytic HMF oxidative reaction（e-HMFOR） have been facing low Faradaic efficiency（FE） and high water splitting ***,we propose a strategy of the NiSeO3@（CoSeO3）4heterojunction by constructing a Co-Ni paired site,where the Co site is in charge of adsorbing for HMF while the electrons are transferred to the Ni site,thus giving the NiSeO3@（CoSeO3）4heterojunction superior electrocata lytic performances for e-HMFOR and water *** optimizing conditions,the NiSeO3@（CoSeO3）4heterojunction has high conversion of 99.7%,high selectivity of 99.9%,and high FE of 98.4% at 1.3 V,as well as low cell voltage of 1.31 V at 10 mA cm-2in 1 M KOH+0.1 M *** study offers a potential insight for e-HMFOR to high value-added FDCA coupling water splitting to produce H2in an economical manner.

关键词： Co-Ni paired site e-HMFOR FDCA Heterojunction Hydrogen evolution

Synergistically enhanced ORR and HER performance on Co-N-C coupled in-situ generated PtCo intermetallic

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Journal of energy chemistry 2025年第1期100卷 721-729页

作者： Guanyu Luo Min Song Lulu An Xiao Huang Qian Zhang Chenhao Zhang Tao Shen Shuang Wang Deli Wang key laboratory of Material chemistry for energy conversion and storage(Huazhong University of Science and Technology)Ministry of Education School of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074HubeiChina

Integrating multi-scale sites in a composite catalyst is vital to realize efficient ***,a synergistic composite catalyst consisting of Co atomic sites and in-situ generated PtCo intermetallic compounds (IMCs)(o-PtCo@CoNC) is proposed through Co pre-anchoring and subsequent impregnation-reduction *** loading of Co atoms provides a chance for in-situ generating PtCo ordered intermetallic *** remaining Co single atoms and PtCo IMCs construct synergistic electrocatalytic *** from the ordered structure,synergistic effect of Pt Co IMCs and Co single atoms,o-PtCo@CoNC exhibits excellent electrocatalytic performance for oxygen reduction reaction (ORR) and hydrogen evolution reaction (HER) with mass activity of 1.21 A mgPt-1(at 0.9 V) and5.70 A mgPt-1(at an overpotential of 100 mV),***,o-PtCo@CoNC delivers negligible loss of half-wave potential and overpotential during long-term stability test in acid solutions,with 13 mV decay after 50,000 potential cycles for ORR and a 2.7 mV decay after 20,000 potential cycles for *** integration strategy of single-atomic sites coupled IMCs paves the way for enhancing the activity and durability of Pt-based electrocatalysts.

关键词： Synergistic effect Intermetallics Single atomic sites Oxygen reduction reaction Hydrogen evolution reaction

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Benchmarking model chemistry composite calculations for vertical ionization potential of molecular systems

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Chinese Chemical Letters 2025年第2期36卷 536-539页

作者： Bingwei Wang Yihong Ding Xiao Tian key laboratory of Carbon materials of Zhejiang Province Wenzhou Key Lab of Advanced Energy Storage and Conversion Zhejiang Province Key Lab of Leather Engineering College of Chemistry and Materials Engineering Wenzhou University laboratory of Theoretical and Computational chemistry Institute of Theoretical Chemistry Jilin University School of Mathematics and Science Hebei GEO University

In chemical science, the vertical ionization potential(VIP) is a crucial metric for understanding the electronegativity, hardness and softness of chemical material systems as well as the electronic structure and stability of molecules. Ever since the last century, the model chemistry composite methods have witnessed tremendous developments in computing the thermodynamic properties as well as the barrier heights. However, their performance in realm of the vertical electron processes of molecular systems has been rarely explored. In this study, we for the first time benchmarked the model chemistry composite methods(e.g., CBS-QB3, G4 and W1BD) in comparison with the commonly used Koopmans' s theorem(KT), electron propagator theory(e.g., OVGF, D2, P3 and P3+) and CCSD(T) methods in calculating the VIP for up to 613 molecular systems with available experimental measurements. The large-scale test calculations strongly showed that the CBS-QB3 model chemistry composite technique can be well recommended to calculate VIP from the perspectives of accuracy, economy and applicability. Notably, the VIP values of up to 7 molecules were identified to have the absolute errors of larger than 0.3 e V at all calculation levels,which have strong hints that their VIP experimental values should be re-investigated.

关键词： CBS-QB3 Composite methods Model chemistry Molecular systems Vertical ionization potential

Development of ESIPT-based specific fluorescent probes for bioactive species based on the protection-deprotection of the hydroxyl

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Chinese Chemical Letters 2025年第2期36卷 49-56页

作者： Haixian Ren Yuting Du Xiaojing Yang Fangjun Huo Le Zhang Caixia Yin Department of chemistry Xinzhou Normal University Research Institute of Applied chemistry Shanxi University Department of chemistry The University of Texas at Austin key laboratory of Chemical Biology and Molecular Engineering of Ministry of Education Key Laboratory of Materials for Energy Conversion and Storage of Shanxi Province Institute of Molecular ScienceShanxi University

Excited-state intramolecular proton-transfer (ESIPT) based fluorescence probes are particularly attractive due to their unique properties including environmental sensitivity, a large Stokes shift, and potential for ratiometric sensing. In general, ESIPT-based fluorophore incorporates an intramolecular hydrogen bonding interaction between a hydrogen bond donor (–OH and NH2are common) and a hydrogen bond acceptor(C=N and C=O). More, protection–deprotection of hydroxyl group as hydrogen bond donor could induce an off-on switch of ESIPT-based emission. Therefore, protection–deprotection of hydroxyl group has been the widely used strategy to design fluorescent probes, where the potential key issue is selecting a protective group that can specifically leave in the presence of the target analyte. In this review, we mainly summarize the specific protecting groups (sites) and deprotection mechanisms for biologically important species (including reactive sulfur species (RSS), reactive oxygen species (ROS), enzymes, etc.), and analyze the advantages and disadvantages of different protection mechanisms from some aspects including probe stability, selectivity, response rate and assay system, etc. Based on the aforementioned, we further point out the current challenges and the potential future direction for developing ESIPT-based probes.

关键词： Bioimaging ESIPT Fluorescence probe Protection-deprotection Specificity

Unraveling the exceptional kinetics of Zn‖organic batteries in hydrated deep eutectic solution

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Journal of energy chemistry 2025年第2期101卷 570-577页

作者： Duo Chen Yuanhang Wang Tengyu Yao Hang Yang Laifa Shen Jiangsu key laboratory of Electrochemical energy storage Technologies College of Materials Science and Technology Nanjing University of Aeronautics and Astronautics Christopher Ingold laboratory Department of Chemistry University College London

Intuitively,the solvation structure featuring stronger interacted sheath in deep eutectic solution（DES）electrolyte would result in sluggish interfacial charge transfer and intense polarization,which obstructs its practical application in emerging Zn based ***,here we discover a Zn‖organic battery with exceptional kinetics properties enabled by a hydrated DES electrolyte,which can render higher discharge capacity,smaller voltage polarization,and faster kinetics of charge transfer in comparison with conventional aqueous 3 M ZnCl2electrolyte,though its viscosity is two orders of magnitude higher than the *** improved kinetics of charge transfer and ion diffusion is demonstrated to originate from the local electron structure regulation of cathode in hydrated DES ***,the DES electrolyte has also been shown to restrict parasitic reaction associated with active water by preferential urea-molecular adsorption on Zn surface and stronger water trapping in solvation structure,giving rise to long-term stable dendrite-free Zn plating/*** work provides a new rationale for understanding electrochemical behaviors of organic cathodes in DES electrolyte,which is conducive to the development of high-performance Zn‖organic batteries.

关键词： Deep eutectic Dendrite-free Kinetics Zn-based battery

Synergistic enhancement of ion/electron transport by ultrafine nanoparticles and graphene in Li2FeTiO4/C/G nanofibers for symmetric Li-ion batteries

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Journal of energy chemistry 2025年第02期101卷 42-51页

作者： Wenjie Ma Yakun Tang Yue Zhang Xiaohui Li Lang Liu Xueting Wang Yuliang Cao State key laboratory of chemistry and Utilization of Carbon Based energy Resources Key Laboratory of Energy Materials Chemistry Ministry of Education College of Chemistry Xinjiang University College of chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power Sources Wuhan University

Low-cost Fe-based disordered rock salt（DRX） Li2FeTiO4is capable of providing high capacity(295 mA h g-1) by redox activity of cations(Fe2+/Fe4+and Ti3+/Ti4+) and anionic ***,DRX structures lack transport channels for ions and electrons,resulting in sluggish kinetics,poor electrochemical activity,and ***,graphene conductive carbon network permeated Li2FeTiO4（LFT/C/G） nanofibers are successfully prepared by a facile sol-gel assisted electrospinning *** Li2FeTiO4nanoparticles（2 nm） and one-dimensional（1D） structure provide abu ndant active sites and unobstructed diffu sion channels,accelerating ion *** addition,introducing graphene reduces the band gap and Li+diffusion barrier and improves the dynamic properties of Li2FeTiO4,thus achieving a relatively mild interfacial reaction and reversible redox *** expected,the LFT/C/1.0G cathode delivers a remarkable discharge capacity(238.5 mA h g-1),high energy density(508.8 Wh kg-1),and excellent rate capability(51.2 mA hg-1at 1.0 A g-1).Besides,the LFT/C/1.0G anode also displays a high capacity(514.5 mA h g-1at 500 mA g-1) and a remarkable rate capability(243.9 mA h g-1at 8 A g-1).Moreover,the full batteries based on the LFT/C/1.0G symmetric electrode demonstrate a reversible capacity of 117.0 mA h g-1after 100 cycles at 50 mA *** study presents useful insights into developing cost-effective DRX cathodes with durable and fast lithium storage.

关键词： 1D structure Disordered rock salt Li2FeTiO4 Graphene Lithium-ion battery electrode Rapid ion/electron transport