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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3期17卷 340-354页

作者： Li An Jianyi Li Yuanmiao Sun Jiamin Zhu Justin Zhu Yeow Seow Hong Zhang Nan Zhang Pinxian Xi * Zhichuan jxu Chun‑Hua Yan State Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceFrontiers Science Center for Rare IsotopesCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000People’s Republic of China School of Materials Science and Engineering Nanyang Technological UniversitySingapore 639798Singapore Faculty of Materials Science and Energy Engineering Institute of Technology for Carbon NeutralityShenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen 518055People’s Republic of China Key Laboratory of Electromagnetic Materials and Devices National Center for International Research On Photoelectric and Energy MaterialsSchool of Materials and EnergyElectron Microscopy CenterYunnan UniversityKunming 650091People’s Republic of China State Key Laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization Baotou Research Institute of Rare EarthsBaotou 014030People’s Republic of China Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU‑HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryPeking UniversityBeijing 100871People’s Republic of China

Water splitting hinges crucially on the availability of electrocatalysts for the oxygen evolution *** surface reconstruction has been widely observed in perovskite catalysts,and the reconstruction degree has been often correlated with the activity ***,a systematic study on the roles of Fe substitution in activation of perovskite LaNiO_(3)is *** substituting Fe content influences both current change tendency and surface reconstruction ***_(0.9)Fe_(0.1)O_(3)is found exhibiting a volcano-peak intrinsic activity in both pristine and reconstructed among all substituted perovskites in the LaNi_(1-x)Fe_(x)O_(3)(x=0.00,0.10,0.25,0.50,0.75,1.00)*** reconstructed LaNi_(0.9)Fe_(0.1)O_(3)shows a higher intrinsic activity than most reported NiFe-based ***,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 ***,it is vital interesting that activity of the reconstructed catalysts relied more on the surface chemistry rather than the reconstruction *** effect of Fe on the degree of surface reconstruction of the perovskite is decoupled from that on its activity enhancement after surface *** 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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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 jxu 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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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 jxu 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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Effects of catalyst mass loading on electrocatalytic activity:An example of oxygen evolution reaction

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Fundamental Research 2021年第4期1卷 448-452页

作者： Linghui Yu Shengnan Suna Haiyan Li Zhichuan jxu School of Materials Science and Engineering Nanyang Technological UniversityBlock N4.150 Nanyang Avenue639798Singapore Singapore-HUJ Alliance for Research and Enterprise Campus for Research Excellence and Technological Enterprise(CREATE)NEW-CREATE Phase II138602Singapore Beijing Innovation Center for Engineering Science and Advanced Technology(BIC-ESAT) Beijing Key Laboratory for Magnetoelectric Materials and Devices(BKL-MMD)School of Materials Science and EngineeringCollege of EngineeringPeking UniversityBeijing 100871China Energy Research Institute@NTU ERI@NInterdisciplinary Graduate SchoolNanyang Technological University639798Singapore

The evaluation of the intrinsic activity of catalysts is the most basic in searching energy-and cost-efficient catalyst materials for various *** accurate determination of the intrinsic activity is essential for identifying efficient *** a huge number of studies of electrocatalysis for various applications have been reported,the effects of electrode loading on the apparent intrinsic activity obtained experimentally have been rarely *** a high mass loading on the electrode,not all the catalyst surfaces can be electrochemically active because not all the surfaces can be wetted by the *** loading also affects the transport of electrons over the electrode as well as the transport of ions in the electrolyte,and thus affects the *** lead to the derivations of the apparent intrinsic activity from the real intrinsic ***,for better understanding the derivations,we evaluate and discuss the effects of electrode mass loading using oxygen evolution reaction as an example.

关键词： Electrocatalysis Water splitting Oxygen reduction reaction Electrode loading

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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 jxu 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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