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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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Molecular ferroelectrics for efficient perovskite solar cells

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Science China Chemistry 2021年第2期64卷 169-170页

作者： chun-hua yan 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 ChemistryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China College of Chemistry and Chemical Engineering Lanzhou UniversityLanzhou 730000China

During the past decade,the power conversion efficiencies(PCEs)of organic-inorganic hybrid perovskite solar cells(PSCs)have exceeded 25%[1],which is expected to be one of the candidates for the next generation of thin-film photovoltaic *** speaking,the performance of PSCs mainly depends on the light absorption capacity,defect passivation and photo-induced exciton separation and extraction of perovskite *** the light illumination,photo-induced excitons were separated and extracted by the built-in electric field of PSCs.

关键词： perovskite illumination inorganic

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Minimum Amount of Extracting Solvent of (A_(1)A_(2)…A_(t−1))/(A_(2)A_(3)…A_(t)) Separation When Using Non-barren Extracting Solvent

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Chinese Journal of Chemistry 2014年第10期32卷 1022-1028页

作者： Fu-Xiang Cheng Sheng Wu Song-Ling Wang Bo Zhang yan Liu chun-Sheng Liao chun-hua yan Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU-HKU Joint Lab on Rare Earth Materials and Bioinorganic ChemistryPeking UniversityBeijing 100871China China Minmetals(Beijing)Research Institute of RE Co. LtdBeijing 100085China

Hyperlink extraction technology,by virtue of its remarkable advantage of decreasing the use of chemicals in multi-component separation,has been extensively employed in rare earth separation industry in *** hyperlink processes,non-barren extracting solvent and scrubbing agent solution which contain the component(s)involved in starting feed are employed in order to save both alkali for saponification and acid for *** amount of extracting solvent(denoted as S_(min))and that of scrubbing agent solution(denoted as W_(min))are important parameters to determine the consumption amounts of alkali and acid for a given countercurrent extraction *** article therefore discusses the influence of using non-barren extracting solvent and scrubbing agent solution on S_(min) and W_(min) of an(A_(1)A_(2)…A_(t−1))/(A_(2)A_(3)…A_(t))*** equations for S_(min) and W_(min) are derived,and the variation of the composition of final raffinate as well as that of final extract are determined,which will provide a valuable guidance for the design of hyperlink extraction processes of multi-component separation,such as rare earths separation.

关键词： minimum amount of extracting solvent rare earths hyperlink process multi-component separation

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Prologue--In memorial to ***-Xian Xu

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Journal of Rare Earths 2017年第1期35卷 I0005-I0006页

作者： chun-hua yan Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistryand Applications PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry College ofChemistry and Molecular Engineering Peking University Beijing 100871 China

Prof. Guang-Xian Xu, the Editor-in-Chief of Journal of the Chinese Society of Rare Earths （JCSRE, in Chinese） and Journal of Rare Earths （JRE, in English）, was a distinguished chemist and educator of China. He was a respected presiding figure in the area of rare earth science in China, and an eminent pioneer in the realm of science, technology and industry of rare earths in the world.

关键词： JRE In memorial to Prof Guang-Xian Xu Prologue

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Boosting the water gas shift reaction on Pt/CeO_(2)-based nanocatalysts by compositional modification: Support doping versus bimetallic alloying

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Journal of Energy Chemistry 2022年第4期31卷 241-249页

作者： Kun Yuan Xiao-Chen Sun Hai-Jing Yin Liang Zhou Hai-Chao Liu chun-hua yan Ya-Wen Zhang Beijing National Laboratory for Molecular Sciences(BNLMS) State Key Laboratory of Rare Earth Materials Chemistry and ApplicationsPKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China Beijing National Laboratory for Molecular Sciences(BNLMS) State Key Laboratory for Structural Chemistry of Stable and Unstable SpeciesCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

The water gas shift reaction is of vital significance for the generation and transition of energy due to the application in hydrogen production and industries such as ammonia synthesis and fuel *** influence of support doping and bimetallic alloying on the catalytic performance of Pt/Ce O_(2)-based nanocatalysts in water gas shift reaction was reported in this *** lanthanide ions and 3d transition metals were respectively introduced into the Ce O_(2)support or Pt to form Pt/Ce O_(2):Ln(Ln=La,Nd,Gd,Tb,Yb)and Pt M/Ce O_(2)(M=Fe,Co,Ni)*** sample of Pt/Ce O_(2):Tb showed the highest activity(TOF at 200℃=0.051 s^(-1))among the Pt/Ce O_(2):Ln and the undoped Pt/Ce O_(2)***,the sample of Pt Fe/Ce O_(2)exhibited the highest activity(TOF at 200℃=0.12 s^(-1))among Pt M/Ce O_(2)*** results of the multiple characterizations indicated that the catalytic activity of Pt/Ce O_(2):Ln catalysts was closely correlated with the amount of oxygen vacancies in doped ceria ***,the different activity of Pt M/Ce O_(2)bimetallic catalysts was owing to the various Pt oxidation states of the bimetals dispersed on *** study of the reaction pathway indicated that both the samples of Pt/Ce O_(2)and Pt/Ce O_(2):Tb catalyzed the reaction through the formate pathway,and the enhanced activity of the latter derived from the increased concentration of oxygen vacancies along with promoted water *** for the sample of Pt Fe/Ce O_(2),its catalytic mechanism was the carboxyl route with a higher reaction rate due to the moderate valence of Pt along with improved CO activation.

关键词： Pt/CeO_(2)catalysts Water–gas shift reaction Support doping Bimetallic alloying

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Stable all-solid-state Li-Te battery with Li_(3)TbBr_(6) superionic conductor

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Nano Research 2023年第7期16卷 9344-9351页

作者： Zhichao Zeng Xiaomeng Shi Mingzi Sun Hongtu Zhang Wei Luo Yunhui huang Bolong huang Yaping Du chun-hua yan Tianjin Key Lab for Rare Earth Materials and Applications Center for Rare Earth and Inorganic Functional MaterialsHaihe Laboratory of Sustainable Chemical TransformationsSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin 300350China Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung HomKowloonHong Kong 999077China Institute of New Energy for Vehicles School of Materials Science and EngineeringTongji UniversityShanghai 201804China Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth MaterialsChemistry and ApplicationsPKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic ChemistryCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China College of Chemistry and Chemical Engineering Lanzhou UniversityLanzhou 730000China

Rare-earth(RE)halide solid electrolytes(HSEs)have been an emerging research area due to their good electrochemical and mechanical properties for all-solid-state lithium batteries(ASSBs).However,only very limited types of HSEs have been reported with high *** this work,tens of grams of RE-HSE Li_(3)TbBr_(6)(LTbB)was synthesized by a vacuum evaporationassisted *** as-prepared LTbB displays a high ionic conductivity of 1.7 mS·cm^(-1),a wide electrochemical window,and good ***,the assembled solid lithium-tellurium(Li-Te)battery based on the LTbB HSE exhibits excellent cycling stability up to 600 cycles,which is superior to most previous *** processes and the chemicals during the discharge/charge of Li-Te batteries have been studied by various in situ and ex situ *** calculations have demonstrated the dominant conductivity contributions of the direct[octahedral]-[octahedral]([Oct]-[Oct])pathway for Li ion migrations in the *** Tb sites guarantee efficient electron transfer while the Li 2s orbitals are not affected during migration,leading to a low activation ***,this successful fabrication and application of LTbB have offered a highly competitive solution for solid electrolytes in ASSBs,indicating the great potential of RE-based HSEs in energy devices.

关键词： rare-earth halide solid electrolytes all-solid-state lithium batteries superionic conductor Li-Te solid battery

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First Binary Mixture Ionic Liquids Containing EMIMBr and IM

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Chinese Chemical Letters 2003年第6期14卷 634-636页

作者： Li Yi DAI chun yan hua Sheng Rong YE Yong Kui SHAN Ming Yuan HE Center for the Chemistry of Ionic Liquid East China Normal UniversityShanghai 200062

A new series of binary mixture ionic liquids comprising 1-ethyl-3-methylimidozalium bromide (EMIMBr) and imidazole (IM) have been synthesized. The melting points of the ionic liquids vary with the different content of IM while they still keep satisfactory conductivity and viscosity. According to the analysis of its phase diagram, the eutectic point is about 16.5C with the mass percentage of IM 29%.

关键词： Ionic liquid binary mixture phase diagram.

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Self-assembly-induced luminescence of Eu3+-complexes and application in bioimaging

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National Science Review 2022年第1期9卷 107-117页

作者： Ping-Ru Su Tao Wang Pan-Pan Zhou Xiao-Xi yang Xiao-Xia Feng Mei-Na Zhang Li-Juan Liang Yu Tang chun-hua yan State Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province College of Chemistry and Chemical Engineering Lanzhou University State Key Laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization Baotou Research Institute of Rare Earths

Design and engineering of highly efficient emitting materials with assembly-induced luminescence,such as room-temperature phosphorescence（RTP） and aggregation-induced emission（AIE）,have stimulated extensive ***,we propose a new strategy to obtain size-controlled Eu;3+;-complex nanoparticles（Eu-NPs） with self-assembly-induced luminescence（SAIL） characteristics without encapsulation or *** with previous RTP or AIE materials,the SAIL phenomena of increased luminescence intensity and lifetime in aqueous solution for the proposed Eu-NPs are due to the combined effe ct of self-assembly in confining the molecular motion and shielding the water *** proof of concept,we also show that this system can be further applied in bioimaging,temperature measurement and HClO *** SAIL activity of the rare-earth（RE） system proposed here offers a further step forward on the roadmap for the development of RE light conversion systems and their integration in bioimaging and therapy applications.

关键词： rare earth complexes self-assembly-induced luminescence bioimaging temperature and HClO sensing

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Multimodal channel cancer chemotherapy by 2D functional gadolinium metal–organic framework

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National Science Review 2021年第7期8卷 175-184页

作者： Jiale Xia Yumeng Xue Bo Lei Lingling Xu Mingzi Sun Na Li Hongyang Zhao Min Wang Meng Luo Chao Zhang Bolong huang Yaping Du chun-hua yan Frontier Institute of Science and Technology Xi'an Jiaotong University Beijing National Laboratory for Molecular Sciences State Key Laboratory of Rare Earth Materials Chemistry and Applications PKU–HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry College of Chemistry and Molecular Engineering Peking University College of Chemistry and Chemical Engineering Lanzhou University Tianjin Key Lab for Rare Earth Materials and Applications School of Materials Science and Engineering National Institute for Advanced Materials Center for Rare Earth and Inorganic Functional Materials Nankai University Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic University

2 D nanomaterials generally exhibit enhanced physiochemical and biological functions in biomedical applications due to their high surface-to-volume ratio and surface charge. Conventional cancer chemotherapy based on nanomaterials has been hindered by their low drug loading and poor penetration in tumor tissue. To overcome these difficulties, novel materials systems are urgently needed. Hereby, the lanthanide-based porphyrin metal–organic framework(MOF) nanosheets(NSs) with promising cancer imaging/chemotherapy capacities are fabricated, which display superior performance in the drug loading and tumor tissue penetration. The biodegradable PPF-Gd NSs deliver an ultrahigh drug loading(>1500%)and demonstrate the stable and highly sensitive stimuli-responsive degradation/release for multimodal tumor imaging and cancer chemotherapy. Meanwhile, PPF-Gd NSs also exhibit excellent fluorescence and magnetic resonance imaging capability in vitro and in vivo. Compared to the traditional doxorubicin(DOX)chemotherapy, the in vivo results confirm the evident suppression of the tumor growth by the PPF-Gd/DOX drug delivery system with negligible side effects. This work further supports the potential of lanthanide-based MOF nanomaterials as biodegradable systems to promote the cancer theranostics technology development in the future.

关键词： lanthanide-based porphyrin metal-organic framework drug delivery stimuli-responsive degradation/release tumor tissue penetration cancer chemotherapy

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Facile synthesis of Au embedded CuOx-CeO2 core/shell nanospheres as highly reactive and sinter-resistant catalysts for catalytic hydrogenation of p-nitrophenol

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Nano Research 2020年第8期13卷 2044-2055页

作者： Ke Wu Xin-Yu Wang Ling-Ling Guo Yue-Jiao Xu Liang Zhou Ze-Yu Lyu Kang-Yu Liu Rui Si Ya-Wen Zhang Ling-Dong Sun chun-hua yan 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 Chemistryand College of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai201204China College of Chemistry and Chemical Engineering Lanzhou UniversityLanzhou730000China

Exploring cost-effective catalysts with high catalytic performance and long-term stability has always been a general concern for environment protection and energy ***,Au nanoparticles(NPs)embedded CuOx-CeO2 core/shell nanospheres(Au@CuOx-CeO2 CSNs)have been successfully prepared through a versatile one-pot method at ambient *** spontaneous auto-redox reaction between HAuCl4 and Ce(OH)3 in aqueous solution triggered the self-assembly growth of micro-/nanostructural Au@CuOx-CeO2 ***,the CuOx clusters in Au@CuOx-CeO2 CSNs are capable of improving the anti-sintering ability of Au NPs and providing synergistic catalysis *** a result,the confined Au NPs exhibited extraordinary thermal stability even at a harsh thermal condition up to 700℃.In addition,before and after the severe calcination process,Au@CuOx-CeO2 CSNs can exhibit enhanced catalytic activity and excellent recyclability towards the hydrogenation of p-nitrophenol compared to previously reported *** synergistic catalysis path between Au/CuOx/CeO2 triphasic interfaces was revealed by density functional theory(DFT)*** CuOx clusters around the embedded Au NPs can provide moderate adsorption strength of p-nitrophenol,while the adjacent CeO2-supported Au NPs can facilitate the hydrogen dissociation to form H*species,which contributes to achieve the efficient reduction of *** study opens up new possibilities for developing high-efficient and sintering-resistant micro-/nanostructural nanocatalysts by exploiting multiphasic systems.

关键词： core/shell nanostructure sinter-resistant catalysts triphasic interfaces catalysis p-nitrophenol reduction

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