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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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Identifying the dynamic behaviors in complete reconstruction of Co-based complex precatalysts during electrocatalytic oxygen evolution

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Journal of Energy Chemistry 2025年第1期100卷 226-233页

作者： Jingfang Zhang Danyang Wu Linke Cai Youluan Lu Fanpeng Cheng Lijuan Shi Qun Yi Yao Liu Yi Huang Key Laboratory of Green Chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education Hubei Key Laboratory of Novel Reactor and Green Chemical Technology School of Chemical Engineering & Pharmacy Wuhan Institute of Technology Key Laboratory of Pesticide & Chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of Education College of Chemistry Central China Normal University College of Materials Science and Engineering Fuzhou University

Transition metal-based nanomaterials have emerged as promising electrocatalysts for oxygen evolution reaction（OER）. Considerable research efforts have shown that self-reconstruction occurs on these nanomaterials under operating conditions of OER process. However, most of them undergo incomplete reconstruction with limited thickness of reconstruction layer, leading to low component utilization and arduous exploration of real catalytic mechanism. Herein, we identify the dynamic behaviors in complete reconstruction of Co-based complexes during OER. The hollow phytic acid（PA） cross-linked CoFe-based complex nanoboxes with porous nanowalls are designed because of their good electrolyte penetration and mass transport ability, in favor of the fast and complete reconstruction. A series of experiment characterizations demonstrate that the reconstruction process includes the fast substitution of PA by OH-to form Co（Fe）(OH)xand subsequent potential-driven oxidation to Co（Fe）OOH. The obtained CoFeOOH delivers a low overpotential of 290 mV at a current density of 10 mA cm-2and a long-term *** experiment results together with theory calculations reveal that the Fe incorporation can result in the electron rearrangement of reconstructed CoFeOOH and optimization of their electronic structure,accounting for the enhanced OER activity. The work provides new insights into complete reconstruction of metal-based complexes during OER and offers guidelines for rational design of high-performance electrocatalysts.

关键词： Oxygen evolution reaction

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Highly mass activity electrocatalysts with ultralow Pt loading on carbon black for hydrogen evolution reaction

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 182-190页

作者： Shaorou Ke Yajing Zhao Xin Min Yanghong Li Ruiyu Mi Yangai Liu Xiaowen Wu Minghao Fang Zhaohui Huang Engineering Research Center of Ministry of Education for Geological Carbon Storage and Low Carbon utilization of resources Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid WastersNational Laboratory of Mineral MaterialsSchool of Materials Science and TechnologyChina University of Geosciences(Beijing)Beijing 100083China

Pt-based nanocatalysts offer excellent prospects for various ***,the low loading of Pt with excellent performance for efficient and stable nanocatalysts still presents a considerable *** this study,nanocatalysts with ultralow Pt content,excellent performance,and carbon black as support were prepared through in-situ ***~2-nm particles uniformly and stably dispersed on carbon black because of the strong s-p-d orbital hybridizations between carbon black and Pt,which suppressed the agglomeration of Pt *** unique structure is beneficial for the hydrogen evolution *** catalysts exhibited remarkable catalytic activity for hydrogen evolution reaction,exhibiting a potential of 100 mV at 100 mA·cm^(-2),which is comparable to those of commercial Pt/C *** activity(1.61 A/mg)was four times that of a commercial Pt/C catalyst(0.37 A/mg).The ultralow Pt loading(6.84wt%)paves the way for the development of next-generation electrocatalysts.

关键词： hydrogen evolution reaction ultralow platinum in-situ synthesis ultrasound

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Effect of pyrite content on chalcopyrite flotation under different regrinding conditions

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 49-57页

作者： Zejun Wang Qing Shi Guofan Zhang Yuxuan Zhu Binbin Li School of Minerals Processing and Bioengineering Central South UniversityChangsha 410083China Key Laboratory of Hunan Province for Clean and Efficient utilization of Strategic Calcium-containing Mineral resources Central South UniversityChangsha 410083China

This study aimed to investigate the effect of varying pyrite(Py)content on copper(Cu)in the presence of different regrinding conditions,which were altered using different types of grinding media:iron,ceramic balls,and their mixture,followed by flotation in the cleaner *** flotation performance of rough Cu concentrate can be improved by changing the regrinding conditions based on the Py *** electron microscopy,X-ray spectrometry,ethylenediaminetetraacetic acid disodium salt extraction,and X-ray photoelectron spectroscopy studies illustrated that when the Py content was high,the use of iron media in regrinding promoted the generation of hydrophilic Fe OOH on the surface of Py and improved the Cu *** ceramic medium with a low Py content prevented excessive Fe OOH from covering the surface of chalcopyrite(Cpy).Electrochemical studies further showed that the galvanic corrosion current of Cpy-Py increased with the addition of Py and became stronger with the participation of iron media.

关键词： chalcopyrite regrinding media pyrite galvanic corrosion flotation

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Synergistic promotion strategy of “dual-site” and “dual-path” to enhance the C–C coupling between CO2 and HCHO driven by photoelectrocatalysis

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Journal of Energy Chemistry 2025年第1期100卷 39-49页

作者： Hongqiang Yang Jianfeng Zheng Guoyu Wang Yifei Gao Yatao Yang Jia Li Xiaojin Han Yan Cui Zhanggen Huang National Key Laboratory of High Efficiency and Low Carbon utilization of Coal Institute of Coal Chemistry Chinese Academy of Science University of Chinese Academy of Science Shenyang University of Chemical Technology

Photoelectrocatalytic coupling CO2and volatile organic compounds （VOCs） is a promising green strategy for the synergistic conversion of the two carbon-containing resources to *** catalytic efficiency is always at the mercy of chemical inertness of CO2and the competitive hydrogen evolution of ***,a modified g-C3N4/ZnAl-LDH Z-scheme heterojunction catalyst with dual reaction site was rationally designed and precisely *** Faraday efficiency of ethanol reached 68.67%with a corresponding formation rate of 227.3μmol *** revealed by in-situ characterizations and density functional theory calculations,CO2and HCHO were absorbed at Zn site and N site,***,*CO generated from CO2and HCHO was converted to*CH3O and*CHO on the dual-active-site *** detailed reaction mechanism experiments indicated that C–C coupling only occurred between*CO and*CH3O in electrocatalysis *** from the“*CO+*CH3O”path,another“*CO+*CHO”coupling path was also detected in photoelectrocatalytic *** selectivity of ethanol was significantly enhanced due to the synthesis of dual-site catalyst and the dual-path coupling path between CO2and HCHO simultaneously driven by light and electricity.

关键词： Ethanol

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Amino acid assisted aqueous synthesis of highly stable CsPbBr_(3)nanocrystals for cell imaging

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Nano Research 2025年第1期18卷 675-683页

作者： Xue Li Yanan Guo Guoying Tan Qingyi Liu Nan Song Yu Tang State Key Laboratory of Applied Organic Chemistry Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu ProvinceCollege of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China State Key Laboratory of Baiyunobo rare earth Resource Researches and Comprehensive utilization Baotou Research Institute of Rare EarthsBaotou 014030China

Lead halide perovskite nanocrystals(NCs)exhibit excellent optoelectronic performance and have drawn great interests in the fields of biological imaging and ***,the poor stability of CsPbX_(3)(X=Cl,Br,I)in water is still a challenge to hinder their practical *** this work,a facile strategy has been developed for aqueous synthesis of CsPbX_(3) nanocrystals,in which L-glutamic acid(LGlu)has been used to replace oleic acid in the synthetic *** from the synergic effects of L-Glu and oleylamine(OAm),CsPbBr_(3)nanocrystals(L-Glu/OAm-CsPbBr_(3)NCs)with high water stability have been directly prepared under a mild condition at room temperature in water,facilitated by the process of crystal phase transformation from Cs_(4)PbBr_(6) to CsPbBr_(3).L-Glu/OAm-CsPbBr_(3)NCs exhibit a high quantum yield of 85%and a narrow full width at half maximum of 16 nm,demonstrating their efficient luminescence in ***,L-Glu on the surface have contributed greatly to an acidic environment and passivation of surface defects,improving the water stability and dispersibility of CsPbBr_(3)***,L-Glu/OAm-CsPbBr_(3)NCs exhibit great biocompatibility due to the presence of L-Glu,resulting in their good performance for HeLa cell ***,we propose a facile and effective method to prepare CsPbBr_(3)nanocrystals with excellent water stability by using L-Glu and OAm as cooperated ligands and expand their application in cell imaging.

关键词： aqueous synthesis cell imaging lead halide perovskite nanocrystals L-glutamic acid phase transformation

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Role of iron ore in enhancing gasification of iron coke:Structural evolution,influence mechanism and kinetic analysis

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 58-69页

作者： Jie Wang Wei Wang Xuheng Chen Junfang Bao Qiuyue Hao Heng Zheng Runsheng Xu School of Chemistry and Materials Science Hubei Engineering UniversityXiaogan 432000China Key Laboratory for Ferrous Metallurgy and resources utilization of Ministry of Education Wuhan University of Science and TechnologyWuhan 430081China Institue of Ironmaking Technology Baosteel Central Research InstituteShanghai 201999China State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China

The utilization of iron coke provides a green pathway for low-carbon *** uncover the influence mechanism of iron ore on the behavior and kinetics of iron coke gasification,the effect of iron ore on the microstructure of iron coke was ***,a comparative study of the gasification reactions between iron coke and coke was conducted through non-isothermal thermogravimetric *** findings indicate that compared to coke,iron coke exhibits an augmentation in micropores and specific surface area,and the micropores further extend and *** provides more adsorption sites for CO_(2) molecules during the gasification process,resulting in a reduction in the initial gasification temperature of iron *** the heating rate in non-isothermal gasification can enhance the reactivity of iron *** metallic iron reduced from iron ore is embedded in the carbon matrix,reducing the orderliness of the carbon structure,which is primarily responsible for the heightened reactivity of the carbon *** kinetic study indicates that the random pore model can effectively represent the gasification process of iron coke due to its rich pore ***,as the proportion of iron ore increases,the activation energy for the carbon gasification gradually decreases,from 246.2 kJ/mol for coke to 192.5 kJ/mol for iron coke 15wt%.

关键词： low-carbon ironmaking iron coke gasification structural evolution kinetic model

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Recovery of vanadium and molybdenum from spent petrochemical catalyst by microwave-assisted leaching

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International Journal of Minerals,Metallurgy and Materials 2019年第1期26卷 33-40页

作者： Zhi-yuan Ma Yong Liu Ji-kui Zhou Mu-dan Liu Zhen-zhen Liu Guangdong institute of resources Comprehensive utilization Guangdong Academy of Sciences State Key Laboratory of Separation and Comprehensive utilization of rare Metals Guangdong Provincial Key Laboratory of development and Comprehensive utilization of Mineral resources

The study of the leaching of vanadium(V) and molybdenum(Mo) from spent petrochemical catalysts in sodium hydroxide(NaO H) medium was performed using two approaches, namely, conventional leaching and microwave-assisted leaching methods. The influence of microwave power, leaching time, leaching temperature, and NaOH concentration on the leaching efficiency of spent petrochemical catalyst was investigated. Under microwave-assisted conditions(600 W, 10 min, 90°C, 2.0 mol·L^(-1) NaOH, and 0.20 g·mL^(-1) solid–liquid ratio), the leaching efficiencies of V and Mo reached 94.35% and 96.23%, respectively. It has been confirmed that microwave energy has considerable potential to enhance the efficiency of the leaching process and reduce the leaching time. It is suggested that the enhancement of the leaching efficiencies of V and Mo can be attributed to the existence of a thermal gradient between solid and liquid and the generation of cracks on the mineral surface.

关键词： microwave spent petrochemical catalyst vanadium molybdenum

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Selective leaching of lithium from spent lithium-ion batteries using sulfuric acid and oxalic acid

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International Journal of Minerals,Metallurgy and Materials 2024年第4期31卷 688-696页

作者： Haijun Yu Dongxing Wang Shuai Rao Lijuan Duan Cairu Shao Xiaohui Tu Zhiyuan Ma Hongyang Cao Zhiqiang Liu institute of Advanced Wear&Corrosion Resistant and Functional Materials Jinan UniversityGuangzhou 510632China institute of resources utilization and rare earth development Guangdong Academy of SciencesGuangzhou 510650China State Key Laboratory of Separation and Comprehensive utilization of rare Metals Guangzhou 510650China Guangdong Province Key Laboratory of rare earth development and Application Guangzhou 510650China

Traditional hydrometallurgical methods for recovering spent lithium-ion batteries(LIBs)involve acid leaching to simultaneously extract all valuable metals into the *** methods usually are followed by a series of separation steps such as precipitation,extraction,and stripping to separate the individual valuable *** this study,we present a process for selectively leaching lithium through the synergistic effect of sulfuric and oxalic *** optimal leaching conditions(leaching time of 1.5 h,leaching temperature of 70°C,liquid-solid ratio of 4 mL/g,oxalic acid ratio of 1.3,and sulfuric acid ratio of 1.3),the lithium leaching efficiency reached89.6%,and the leaching efficiencies of Ni,Co,and Mn were 12.8%,6.5%,and 21.7%.X-ray diffraction(XRD)and inductively coupled plasma optical emission spectrometer(ICP-OES)analyses showed that most of the Ni,Co,and Mn in the raw material remained as solid residue oxides and *** study offers a new approach to enriching the relevant theory for selectively recovering lithium from spent LIBs.

关键词： selective leaching oxalic acid sulfuric acid spent lithium-ion batteries

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Metallurgical properties of CaO–SiO_(2)–Al_(2)O_(3)–4.6wt%MgO–Fe_(2)O_(3)slag system pertaining to spent automotive catalyst smelting

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International Journal of Minerals,Metallurgy and Materials 2023年第5期30卷 886-896页

作者： Ruili Zheng Jianfang Lü Weifeng Song Mudan Liu Huashan Li Yong Liu Xianjin Lü Zhiyuan Ma School of Environmental Science and Engineering Guangdong University of TechnologyGuangzhou 510006China institute of resources utilization and rare earth development Guangdong Academy of SciencesGuangzhou 510650China State Key Laboratory of rare Metals Separation and Comprehensive utilization Guangzhou 510650China Guangdong Key Laboratory of Mineral resources development and Comprehensive utilization Guangzhou 510650China

The metallurgical properties of the CaO–SiO_(2)–Al_(2)O_(3)–4.6wt%Mg O–Fe_(2)O_(3)slag system,formed by the co-treatment process of spent automotive catalyst(SAC)and copper-bearing electroplating sludge(CBES),were studied systematically in this *** slag structure,melting temperature,and viscous characteristics were investigated by Fourier transform infrared(FTIR)spectroscopy,Raman spectroscopy,Fact Sage calculation,and viscosity *** results show that the increase of Fe_(2)O_(3)content(3.8wt%–16.6wt%),the mass ratio of CaO/SiO_(2)(m(CaO)/m(SiO_(2)),0.5–1.3),and the mass ratio of SiO_(2)/Al_(2)O_(3)(m(SiO_(2))/m(Al_(2)O_(3)),1.0–5.0)can promote the depolymerization of silicate network,and the presence of a large amount of Fe_(2)O_(3)in form of tetrahedral and octahedral units ensures the charge compensation of Al^(3+)ions and makes Al_(2)O_(3)only behave as an acid *** calculation and viscosity measurements show that with the increase of Fe_(2)O_(3)content,m(Ca O)/m(SiO_(2)),and m(SiO_(2))/m(Al_(2)O_(3)),the depolymerization of silicate network structure and low-melting-point phase transformation first occur within the slag,leading to the decrease in melting point and viscosity of the slag,while further increase causes the formation of high-melting-point phase and a resultant re-increase in viscosity and melting *** on experimental analysis,the preferred slag composition with low polymerization degree,viscosity,and melting point is as follows:Fe_(2)O_(3)content of 10.2wt%–13.4wt%,m(CaO)/m(SiO_(2))of 0.7–0.9 and m(SiO_(2))/m(Al_(2)O_(3))of 3.0–*** work provides a theoretical support for slag design in co-smelting process of SAC and CBES.

关键词： spent automotive catalyst co-treatment slag system slag structure melting temperature phase transformation viscosity

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