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Deciphering Water Oxidation Catalysts: The Dominant Role of Surface Chemistry over Reconstruction Degree in Activity Promotion

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NANO-MICRO LETTERS 2025年第1期17卷 1-15页

作者： An, Li Li, jianyi Sun, Yuanmiao Zhu, jiamin Seow, justin Zhu Yeow Zhang, Hong Zhang, Nan Xi, Pinxian Xu, zhichuan j. Yan, Chun-Hua Lanzhou univ Frontiers Sci Ctr Rare Isotopes Key Lab Nonferrous Met Chem & Resources Utilizat G State Key Lab Appl Organ ChemColl Chem & Chem Eng Lanzhou 730000 Peoples R China Nanyang Technol univ Sch Mat Sci & Engn Singapore 639798 Singapore Chinese Acad Sci Fac Mat Sci & Energy Engn Shenzhen Inst Adv Technol Inst Technol Carbon Neutral Shenzhen 518055 Peoples R China Yunnan univ Natl Ctr Int Res Photoelect & Energy Mat Electron Microscopy Ctr Sch Mat & EnergyKey Lab Electromagnet Mat & Devic Kunming 650091 Peoples R China Baotou Res Inst Rare Earths State Key Lab Baiyunobo Rare Earth Resource Res & Baotou 014030 Peoples R China Peking univ Beijing Natl Lab Mol Sci State Key Lab Rare Earth Mat Chem & Applicat PKU HKU Joint Lab Rare Earth Mat & Bioinorgan Chem Beijing 100871 Peoples R China

Demonstrate that the key factor to determine the activity of reconstructed surfaces is the surface chemistry, instead of reconstruction degree using the popular perovskite LaNi1-xFexO3 oxides as model *** content can influence both the surface reconstruction degree, the activation degree, and the activity of reconstructed *** oxygen evolution reaction activity of reconstructed catalysts is primarily governed by the chemistry of the reconstructed surface species. Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution reaction. The surface reconstruction has been widely observed in perovskite catalysts, and the reconstruction degree has been often correlated with the activity enhancement. Here, a systematic study on the roles of Fe substitution in activation of perovskite LaNiO3 is reported. The substituting Fe content influences both current change tendency and surface reconstruction degree. LaNi0.9Fe0.1O3 is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi1-xFexO3 (x = 0.00, 0.10, 0.25, 0.50, 0.75, 1.00) series. The reconstructed LaNi0.9Fe0.1O3 shows a higher intrinsic activity than most reported NiFe-based catalysts. Besides, density functional theory calculations reveal that Fe substitution can lower the O 2p level, which thus stabilize lattice oxygen in LaNi0.9Fe0.1O3 and ensure its long-term stability. Furthermore, it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction degree. The effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface reconstruction. This finding showcases the importance to customize the surface chemistry of reconstructed catalysts for water oxidation.

关键词： Oxygen evolution reaction Perovskite oxides Doping Activation and reconstruction

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From Two-Phase to Three-Phase: The New Electrochemical Interface by Oxide Electrocatalysts

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Nano-Micro Letters 2018年第1期10卷 74-76页

作者： zhichuan j.Xu School of Materials Science and Engineering Nanyang Technological University Solar Fuels Lab Nanyang Technological University Energy Research Institute NTu (ERIN) Nanyang Technological University

Electrochemical reactions typically occur at the interface between a solid electrode and a liquid electrolyte. The charge exchange behaviour between these two phases determines the kinetics of electrochemical reactions. In the past few years, significant advances have been made in the development of metal oxide electrocatalysts for fuel cell and electrolyser reactions. However, considerable gaps remain in the fundamental understanding of the charge transfer pathways and the interaction between the metal oxides and the conducting substrate on which they are located. In particular, the electrochemical interfaces of metal oxides are significantly different from the traditional(metal) ones, where only a conductive solid electrode and a liquid electrolyte are considered. Oxides are insulating and have to be combined with carbon as a conductive *** electrode configuration results in a three-phase electrochemical interface, consisting of the insulating oxide, the conductive carbon, and the liquid electrolyte. To date, the mechanistic insights into this kind of non-traditional electrochemical interface remain unclear. Consequently conventional electrochemistry concepts, established on classical electrode materials and their two-phase interfaces, are facing challenges when employed for explaining these new electrode materials.

关键词： Electrochemistry Interface Oxides Carbon Electrocatalyst

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Electrodeposited Sulfur and CoxS Electrocatalyst on Buckypaper as High-Performance Cathode for Li-S Batteries

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Nano-Micro Letters 2020年第10期12卷 263-275页

作者： Yi Zhan Andrea Buffa Linghui Yu zhichuan j.u Daniel Mandler School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore Institute of Chemistry The Hebrew University of Jerusalem9190401 JerusalemIsrael Campus for Research Excellence and Technological Enterprise(CREATE) Singapore-HUJ Alliance for Research and Enterprise(SHARE)Singapore 138602Singapore

Lithium-sulfur batteries(LSBs)are considered as the next generation of advanced rechargeable batteries because of their high energy *** this study,sulfur and CoxS electrocatalyst are deposited on carbon nanotube buckypaper(S/CoxS/BP)by a facile electrodeposition method and are used as a binder-free high-performance cathode for *** sulfur is deposited on buckypaper by electrooxidation of a polysulfide solution(-S6^2-).This approach substantially increased the current and time efficiency of sulfur electrochemical deposition on conductive material for LSBs.S/CoxS/BP cathode could deliver an initial discharge capacity as high as 1650 mAh g^-1 at 0.1 C,which is close to the theoretical capacity of *** current rate of 0.5 C,the S/CoxS/BP has a capacity of 1420 mAh g^-1 at the first cycle and 715 mAh g^-1 after 500 cycles with a fading rate of 0.099%per *** high capacity of S/CoxS/BP is attributed to both the homogeneous dispersion of nanosized sulfur within BP and the presence of CoxS *** sodium dodecyl sulfate(SDS)pretreatment of BP renders it polarity to bind polysulfides and thus facilitates the good dispersibility of nanosized sulfur within *** catalyst accelerates the kinetics of polysulfide conversion and reduces the presence of polysulfide in the cathode,which suppresses the polysulfide diffusion to anode,i.e.,the shuttle *** mitigation of the active material loss improves not only the capacity but also the cyclability of S/CoxS/BP.

关键词： Electrodeposition Lithium sulfur batteries Buckypaper Electrocatalysts

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A new insight into electrochemical detection of eugenol by hierarchical sheaf-like mesoporous NiCo2O4

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Nano Research 2015年第8期8卷 2636-2645页

作者： Mylamparambil udayan Anu Prathap Chao Wei Shengnan Sun zhichuan j. Xu School of Materials Science and Engineering Nanyang Technological University 50 Nanyang Avenue Singapore 639798 Singapore

NiCo2O4 nanosheets with sheaf-like nanostructure morphologies have been synthesized by a facile one-step hydrothermal reaction followed by annealing treatment. Impressively, the NiCo2O4 nanosheets exhibit rapid detection of eugenol. The linear range of detection is from 1-500μM, and the limit of detection is 5.4 μM. The NiCo2O4 modified electrode demonstrated high sensitivity, good repeatability and reproducibility, and long-term stability （7% decrease in response over 30 days）. Based on this work, an electrochemical reaction mechanism for eugenol oxidation was proposed, and in addition, the NiCo2O4 modified electrode was successfully employed for the analysis of eugenol in medicative balm samples. Recovery values for eugenol in medicative balm samples were in the range 98.7%-105.5%.

关键词： NiCo2O4 nanosheets eugenol determination electrocatalysis electrochemical mechanism real sample analysis

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A Flexible and Lightweight Biomass-Reinforced Microwave Absorber

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Nano-Micro Letters 2020年第10期12卷 1-15页

作者： Yan Cheng justin Zhu Yeow Seow Huanqin Zhao zhichuan j.u Guangbin ji College of Materials Science and Technology Nanjing University of Aeronautics and AstronauticsNanjing 210016People’s Republic of China School of Materials Science and Engineering Nanyang Technological University50 Nanyang AvenueSingapore 639798Singapore Singapore-Huj Alliance for Research and Enterprise NEW-CREATE PhaseⅡCampus for Research Excellence and Technological Enterprise(CREATE)Singapore 138602Singapore

Developing a flexible,light-weight and effective electromagnetic(EM)absorber remains challenging despite being on increasing demand as more wearable devices and portable electronics are ***,we report a flexible and lightweight hybrid paper by a facile vacuumfiltration-induced self-assembly process,in which cotton-derived carbon fibers serve as flexible skeletons,compactly surrounded by other microwave-attenuating components(reduced graphene oxide and Fe3O4@C nanowires).Owing to its unique architecture and synergy of the three components,the asprepared hybrid paper exhibits flexible and lightweight features as well as superb microwave absorption *** absorption intensity with reflection loss as low as-63 dB can be achieved,and its broadest frequency absorption bandwidth of 5.8 GHz almost covers the entire Ku *** a hybrid paper is promising to cope with ever-increasing EM *** work also paves the way to develop low-cost and flexible EM wave absorber from biomass through a facile method.

关键词： Flexible Biomass Microwave absorption Dielectric loss Magnetic loss

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In Situ X-ray Absorption Spectroscopy Studies of Nanoscale Electrocatalysts

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Nano-Micro Letters 2019年第3期11卷 178-195页

作者： Maoyu Wang Líneyárnadóttir zhichuan j.u Zhenxing Feng School of Chemical Biologicaland Environmental EngineeringOregon State UniversityCorvallisOR97331USA School of Materials Science and Engineering Nanyang Technological UniversitySingapore639798Singapore

Nanoscale electrocatalysts have exhibited promising activity and stability,improving the kinetics of numerous electrochemical reactions in renewable energy systems such as electrolyzers,fuel cells,and metal-air *** to the size effect,nano particles with extreme small size have high surface areas,complicated morphology,and various surface terminations,which make them different from their bulk phases and often undergo restructuring during the *** restructured materials are hard to probe by conventional ex-situ characterizations,thus leaving the true reaction centers and/or active sites difficult to ***,in situ techniques,particularly X-ray absorption spectroscopy(XAS),have become an important tool to obtain oxidation states,electronic structure,and local bonding environments,which are critical to investigate the electrocatalysts under real reaction *** this review,we go over the basic principles of XAS and highlight recent applications of in situ XAS in studies of nanoscale electrocatalysts.

关键词： X-ray absorption spectroscopy Electrocatalyst Nanoscale In situ experiments

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Trifluoromethoxylation/trifluoromethylthiolation/trifluoromethylselenolation strategy for the construction of heterocycles

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Chinese Chemical Letters 2023年第5期34卷 3-15页

作者： Xin Wang zhichuan Wang Zhenjian Li Kai Sun College of Chemistry and Chemical Engineering Yantai UniversityYantai 264005China State Key Laboratory of Tree Genetics and Breeding Research Institute of ForestryChinese Academy of ForestryBeijing 100091China

The XCF_(3)groups(X=O,S,Se)play an increasingly important role in modern organic chemistry due to their unique electronegativity,lipophilic nature,metabolic stability,and *** compounds are important scaffolds in many bioactive compounds and *** incorporation of XCF_(3)groups into heterocyclic compounds can change their physicochemical and biological properties,which injects new vitality into the application of heterocyclic compounds in many fields such as organic chemistry,the pharmaceutical chemistry,and life *** this paper,the recent progress in the synthesis of F_(3)CX-containing heterocycles is reviewed,and the application scope and mechanism of some reactions are discussed.

关键词： Trifluoromethoxylation Trifluoromethylthiolation Trifluoromethylselenolation Cyclization

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Carbon-Nitride-Based Materials for Advanced Lithium-Sulfur Batteries

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Nano-Micro Letters 2022年第12期14卷 579-601页

作者： Wenhao Sun Zihao Song Zhenxing Feng Yaqin Huang zhichuan j.Xu Yi-Chun Lu Qingli Zou State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China Electrochemical Energy and Interfaces Laboratory Department of Mechanical and Automation EngineeringThe Chinese University of Hong KongHong Kong Special Administrative Region 999077People’s Republic of China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Republic of Singapore School of Chemical Biologicaland Environmental EngineeringOregon State UniversityCorvallisOR 97331USA

Lithium-sulfur(Li-S)batteries are promising candidates for next-generation energy storage systems owing to their high energy density and low ***,critical challenges including severe shuttling of lithium polysulfides(LiPSs)and sluggish redox kinetics limit the practical application of Li-S *** nitrides(C_(x)N_(y)),represented by graphitic carbon nitride(g-C_(3)N_(4)),provide new opportunities for overcoming these *** a graphene-like structure and high pyridinic-N content,g-C_(3)N_(4) can effectively immobilize LiPSs and enhance the redox kinetics of S *** addition,its structure and properties including electronic conductivity and catalytic activity can be regulated by simple methods that facilitate its application in Li-S ***,the recent progress of applying C_(x)N_(y)-based materials including the optimized g-C_(3)N_(4),g-C_(3)N_(4)-based composites,and other novel C_(x)N_(y) materials is systematically reviewed in Li-S batteries,with a focus on the structure-activity *** limitations of existing C_(x)N_(y)-based materials are identified,and the perspectives on the rational design of advanced C_(x)N_(y)-based materials are provided for high-performance Li-S batteries.

关键词： Lithium-sulfur batteries Carbon nitride Polysulfide conversion Shuttle effect Anode protection

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Transition metal oxides for water oxidation: All about oxyhydroxides?

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Science China Materials 2020年第1期63卷 3-7页

作者： zhichuan j.Xu School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore Energy Research Institute NTu ERI NInterdisciplinary Graduate SchoolNanyang Technological UniversitySingapore 639798Singapore Solar Fuels Lab Nanyang Technological UniversitySingapore 639798Singapore The Cambridge Centre for Advanced Research and Education in Singapore Singapore 138602Singapore

To realize a sustainable hydrogen energy infrastructure,techniques to produce hydrogen gas without involving fossil fuels are *** has been proposed in last century that producing hydrogen gas by splitting water could ... 详细信息

关键词：氧化物催化剂过渡金属氧化物活性表面氢氧化物析氧反应表面重构电解水催化剂表面

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The possible implications of magnetic field effect on understanding the reactant of water splitting

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Chinese j.urnal of Catalysis 2022年第1期43卷 148-157页

作者： Chao Wei zhichuan j.Xu School of Materials Science and Engineering Nanyang Technological UniversitySingapore Energy Research Institute Nanyang Technological UniversitySingapore Singapore‐Huj Alliance for Research and Enterprise NEW‐CREATE Phase IICampus for Research Excellence and Technological Enterprise(CREATE)Singapore

Electrochemical water splitting consists of two elementary reactions i.e.,hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Developing robust HER and OER technologies necessitates a molecular picture of reaction mechanism,yet the reactants for water splitting reactions are unfortunately not fully *** we utilize magnetic field to understand proton transport in HER,and hydroxide ion transport in OER,to discuss the possible implications on understanding the reactants for HER and *** field is a known tool for changing the movement of charged species like ions,*** magnetic‐field‐improved Cu^(2+)transportation near the electrode in Cu ***,applying a magnetic field does not affect the HER or OER rate across various pH,which challenges the traditional opinion that charged species(*** and hydroxide ion)act as the *** anomalous response of HER and OER to magnetic field,and the fact that the transport of proton and hydroxide ion follow Grotthuss mechanism,collectively indicate water may act as the universal reactant for HER and OER across various *** the aid of magnetic field,this work serves as an understanding of water might be the reactant in HER and OER,and possibly in other electrocatalysis reactions involving protonation and deprotonation step.A model that simply focuses on the charged species but overlooking the complexity of the whole electrolyte phase where water is the dominant species,may not reasonably reflect the electrochemistry of HER and OER in aqueous electrolyte.

关键词： Electrocatalysis Water splitting Magnetic field Lorenz force Metal deposition

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