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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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Electronic structure and flotability of gold-bearing pyrite:A density functional theory study

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Journal of Central South University 2017年第10期24卷 2288-2293页

作者： LIU Dan WANG Yi-jie XIAN Yong-jun WEN Shu-ming State key laboratory of complex nonferrous Metal Resources clean utilization(Kunming University of Science and Technology) Kunming 650093China

Various incorporation of Au in pyrite and its effects on the geometrical structure,electronic structure and flotability of pyrite were theoretically investigated and fully discussed by performing density functional theory(DFT).The calculated incorporation energy shows that gold would most likely exist in pyrite via incorporating into interstitial lattice sites in the absence of As *** a result of incorporated Au,the covalence levels of the S—Fe and S—S bonds are changed,and the tonicity of Au—S bonds and antibonding of Au—Fe bonds are found to form in the pyrite,which would change the natural flotability of *** Au impurity energy levels are introduced into the energy band and result in the transformation of pyrite semiconductivity *** calculated band-gap value suggests that the incorporated Au significantly decreases pyrite semiconductivity level,which enhances the formation and the adsorption stability of dixanthogen during pyrite *** DOS results reveal that the stability and depression difficulty level of pyrites increases in the following order:Fe_(32)S_(63)As

关键词： pyrite gold density functional theory electronic structure flotability

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Extracting copper from copper oxide ore by a zwitterionic reagent and dissolution kinetics

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International Journal of Minerals,Metallurgy and Materials 2015年第3期22卷 241-248页

作者： Jiu-shuai Deng Shu-ming Wen Jian-ying Deng Dan-dan Wu State key laboratory of complex nonferrous Metal Resources clean utilization Faculty of Land Resource Engineering Kunming University of Science and Technology

Sulfamic acid （SA）, which possesses a zwitterionic structure, was applied as a leaching reagent for the first time for extracting copper from copper oxide ore. The effects of reaction time, temperature, particle size, reagent concentration, and stirring speed on this leach- ing were studied. The dissolution kinetics of malachite was illustrated with a three-dimensional diffusion model. A novel leaching effect of SA on malachite was eventually demonstrated. The leaching rate increased with decreasing particle size and increasing concentration, reac- tion temperature and stirring speed. The activation energy for SA leaching malachite was 33.23 kJ/mol. Furthermore, the effectiveness of SA as a new reagent for extracting copper from copper oxide ore was confirmed by experiment. This approach may provide a solution suitable for subsequent electrowinning. In addition, results reported herein may provide basic data that enable the leaching of other carbonate miner- als of copper, zinc, cobalt and so on in an SA system.

关键词： malachite copper extraction sulfamic acid dissolution kinetics

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A novel method for improving cerussite sulfidization

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International Journal of Minerals,Metallurgy and Materials 2016年第6期23卷 609-617页

作者： Qi-cheng Feng Shu-ming Wen Wen-juan Zhao Qin-bo Cao Chao Lü State key laboratory of complex nonferrous Metal Resources clean utilization Kunming University of Science and Technology Kunming Metallurgical Research Institute

Evaluation of flotation behavior, solution measurements, and surface analyses were performed to investigate the effects of chloride ion addition on the sulfidization of cerussite in this study. Micro-flotation tests indicate that the addition of chloride ions prior to sulfidization can significantly increase the flotation recovery of cerussite, which is attributed to the formation of more lead sulfide species on the mineral surface. Solution measurement results suggest that the addition of chloride ions prior to sulfidization induces the transformation of more sulfide ions from pulp solution onto the mineral surface by the formation of more lead sulfide species. X-ray diffraction and energy-dispersive spectroscopy indicate that more lead sulfide species form on the mineral surface when chloride ions are added prior to sulfidization. These results demonstrate that the addition of chloride ions prior to sulfidization can significantly improve the sulfidization of cerussite, thereby enhancing the flotation performance.

关键词： cerussite sulfidization chloride surface analysis

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Morphology and activity relationships of macroporous CuO-ZnO-ZrO_2 catalysts for methanol synthesis from CO_2 hydrogenation

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Rare Metals 2016年第10期35卷 790-796页

作者： Yu-Hao Wang Wen-Gui Gao Hua Wang Yan-E Zheng Kong-Zhai Li Ru-Gui Ma State key laboratory of complex nonferrous Metal Resources clean utilization Engineering Faculty of Metallurgy and Energy EngineeringKunming University of Science and Technology

A series of macroporous CuO-ZnO-ZrO2 （CZZ） catalysts with different Zn/Zr ratios were successfully prepared by template method and characterized by X-ray diffraction （XRD）, N2 adsorption, reactive N2O adsorption, scanning electron microscopy （SEM）, H2 temperature-pro- grammed reduction （H2-TPR）, and transmission electron microscopy （TEM）. The activity of the catalysts was tested for methanol synthesis from CO2 hydrogenation. It is found that the increase in the Zn/Zr ratio could lead to the sintering of the catalysts, destroying the macroporous structure integrity. The macroporous CZZ catalysts own lower Zn/Zr ratio, exhibiting a better morphology and activity. For comparison, the conventional nonporous CZZ catalysts were also investigated. The results show that the CZZ catalysts with macroporous structure own smaller particles, higher CO2 conversion, and CH3OH yield. It reveals that the macroporous structure could inhibit the growth of the par- ticle size, and the special porous structure is favorable for diffusion and penetration of CO2, which could improve the catalytic activities.

关键词： Macroporous structure CuO-ZnO-ZrO2 catalysts CO2 hydrogenation Methanol Activity

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New influence factor inducing difficulty in selective flotation separation of Cu–Zn mixed sulfide minerals

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International Journal of Minerals,Metallurgy and Materials 2015年第2期22卷 111-115页

作者： Jiu-shuai Deng Ying-bo Mao Shu-ming Wen Jian Liu Yong-jun Xian Qi-cheng Feng State key laboratory of complex nonferrous Metal Resources clean utilization Faculty of Land Resource Engineering Kunming University of Science and Technology

Selective flotation separation of Cu-Zn mixed sulfides has been proven to be difficult. Thus far, researchers have found no satis- factory way to separate Cu-Zn mixed sulfides by selective flotation, mainly because of the complex surface and interface interaction mecha- nisms in the flotation solution. Undesired activation occurs between copper ions and the sphalerite surfaces. In addition to recycled water and mineral dissolution, ancient fluids in the minerals are observed to be a new source of metal ions. In this study, significant amounts of ancient fluids were found to exist in Cu-Zn sulfide and gangue minerals, mostly as gas-liquid fluid inclusions. The concentration of copper ions re- leased from the ancient fluids reached 1.02 × 10-6 tool/L, whereas, in the cases of sphalerite and quartz, this concentration was 0.62 ×10-6 mol/L and 0.44 × 10-6 mol/L, respectively. As a result, the ancient fluid is a significant source of copper ions compared to mineral dissolution under the same experimental conditions, which promotes the unwanted activation of sphalerite. Therefore, the ancient fluid is considered to be a new factor that affects the selective flotation separation of Cu-Zn mixed sulfide ores.

关键词： sulfide minerals flotation separation fluid inclusions

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Sulfidization regulation of cuprite by pre-oxidation using sodium hypochlorite as an oxidant

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International Journal of Mining Science and Technology 2021年第6期31卷 1117-1128页

作者： Guang Han Shuming Wen Han Wang Qicheng Feng State key laboratory of complex nonferrous Metal Resources clean utilization Faculty of Land Resources EngineeringKunming University of Science and TechnologyKunming 650093China

The direct sulfidization of cuprite is inefficient because cuprite is a copper-oxide mineral with a strong surface *** this study,oxidant was used to modify cuprite surfaces to regulate the sulfidization of *** tests showed that the flotation recovery of pre-oxidized cuprite was nearly25% higher than that of direct sulfidization flotation,which indicates that the cuprite surface activity was enhanced after pre-oxidation by Cu(Ⅰ) species(weak affinity with sulfur ions) transformation to Cu(Ⅱ)species(strong affinity with sulfur ions).Zeta potential,scanning electron microscopy-energy dispersive X-ray spectroscopy,X-ray photoelectron spectroscopy,and time-of-flight secondary ion mass spectrometry results showed that pre-oxidation improved cuprite sulfidization and promoted the formation of copper-sulfide species on the cuprite *** mineral surface stability and thus,xanthate species adsorption on the cuprite surfaces were *** surface-adsorption measurements and infrared spectroscopy showed that a large amount of xanthate species was adsorbed onto the sulfidized cuprite surfaces after pre-oxidation,which enhanced the cuprite hydrophobicity and improved the cuprite flotation.

关键词： Cuprite Pre-oxidation Enhanced sulfidization Xanthate adsorption

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Analysis of Crystallization Behavior of Mold Fluxes Containing TiO_2 Using Single Hot Thermocouple Technique

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Journal of Iron and Steel Research International 2016年第4期23卷 322-328页

作者： Yun LEI Bing XIE Wen-hui MA State key laboratory of complex nonferrous Metal Resources clean utilization Kunming University of Science and Technology College of Materials Science and Engineering Chongqing University

The crystallization behavior of mold fluxes containing 0-8 mass% TiO2 was investigated using the single hot therrnocouple technique （SHTT） and X ray diffraction （XRD） to study the possible effects on the coordination of heat transfer control and strand lubrication for casting crack sensitive peritectic steels. Time-temperature-transforma tion （TTT） and continuous-cooling transformation （CCT） curves were plotted using the data obtained from SHTT to characterize the crystallization of the mold fluxes. The results showed that crystallization of the mold fluxes during isothermal and non-isothermal processes was suppressed with TiO2 addition. From the TTT curves, it could be seen that the incubation and growth time of crystallization increased significantly with TiO2 addition. The CCT curves showed that the crystallization temperature initially decreased, and then suddenly increased with increasing the TiO2 content. XRD analysis suggested the presence of cuspidine in the mold fluxes with lower TiO2 content （〈4 mass%） , while both perovskite and cuspidine were detected in the mold fluxes when the TiO2 content was increased to 8 mass%. In addition, the growth mechanisms of the crystals changed during the isothermal crystallization process from interface controlled growth to diffusion-controlled growth with increasing the TiO2 content.

关键词： mold flux single hot thermocouple technique kinetics crystallization TTT curve CCT curve

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Oxygen vacancies enriched Ni-Co/SiO_(2)@CeO_(2) redox catalyst for cycling methane partial oxidation and CO_(2) splitting

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Chinese Journal of Chemical Engineering 2023年第11期63卷 235-245页

作者： Chang Yang Juping Zhang Jiakai Wang Dongfang Li Kongzhai Li Xing Zhu State key laboratory of complex nonferrous Metal Resources clean utilization Faculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093China

Redox catalysts play a vital role in the interconversion of two significant greenhouse gases,CO_(2)and CH_(4),via chemical looping methane dry reforming ***,a series of transition metals-alloyed and core-shell structured Ni-M/SiO_(2)@CeO_(2)(M=Fe,Co,Cu,Mn,Zr)redox catalyst were fabricated and evaluated in a gas-solid fixed-bed reactor for cycling CH_(4)partial oxidation(PO_(x))and CO_(2)*** catalysts are composed of spherical SiO_(2)core and CeO_(2)shell,and the highly dispersed Ni alloy nanoparticles are the interlayer between core and *** oxygen vacancy concentration of Ni-M/SiO_(2)@CeO_(2)followed the order of Co>Cu>Fe>Mn>Zr,and Ni alloying with transition metals significantly enhanced oxygen storage capacity(OSC).Ni-Co/SiO_(2)@CeO_(2)catalyst with abundant oxygen vacancies and a high OSC showed the lowest temperatures of CH_(4)activation(610℃)and CO_(2)decomposition(590℃),thus demonstrating excellent redox *** catalyst exhibited superior activity and structural stability in the continuous CH_(4)/CO_(2)redox cycles at 615℃,achieving 87%CH_(4)conversion and 83%CO *** proposed catalyst shows great potential for the utilization of CH_(4)and CO_(2)in a redox mode,providing a new sight for design redox catalyst in chemical looping or related fields.

关键词： Chemical looping Methane Dry reforming Catalyst Partial Oxidation

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Thermodynamic theory of flotation for a complex multiphase solid -liquid system and high-entropy flotation

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International Journal of Minerals,Metallurgy and Materials 2024年第6期31卷 1177-1197页

作者： Shuming Wen State key laboratory of complex nonferrous Metal Resources clean utilization Faculty of Land Resource EngineeringKunming University of Science and TechnologyKunming 650093China

The flotation of complex solid–liquid multiphase systems involve interactions among multiple components,the core problem facing flotation ***,the combined use of multicomponent flotation reagents to improve mineral flotation has become an important issue in studies on the efficient use of refractory mineral ***,studying the flotation of complex solid–liquid systems is extremely difficult,and no systematic theory has been developed to *** addition,the physical mechanism associated with combining reagents to improve the flotation effect has not been unified,which limits the development of flotation theory and the progress of flotation *** this study,we applied theoretical thermodynamics to a solid–liquid flotation system and used changes in the entropy and Gibbs free energy of the reagents adsorbed on the mineral surface to establish thermodynamic equilibrium equations that de-scribe interactions among various material components while also introducing adsorption equilibrium constants for the flotation reagents adsorbed on the mineral *** homogenization effect on the mineral surface in pulp solution was determined using the chemical potentials of the material components of the various mineral surfaces required to maintain *** flotation effect can be improved through synergy among multicomponent flotation reagents;its physical essence is the thermodynamic law that as the number of compon-ents of flotation reagents on the mineral surface increases,the surface adsorption entropy change increases,and the Gibbs free energy change of adsorption *** to the results obtained using flotation thermodynamics theory,we established high-entropy flotation theory and a technical method in which increasing the types of flotation reagents adsorbed on the mineral surface,increasing the adsorption entropy change of the flotation reagents,decreasing the Gibbs free energy change,and improving the adsorption efficiency

关键词： multicomponent flotation reagent adsorption entropy change equations of thermodynamic equilibrium adsorption equilibri-um constant high-entropy flotation

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