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Achievable dual-strategy to stabilize Li-rich layered oxide interface by a one-step wet chemical reaction towards long oxygen redox reversibility

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Journal of energy Chemistry 2025年第2期101卷 120-131页

作者： Bin He Yujie Dai Shuai Jiang Dawei Chen Xilong Wang Jie Song Dan Xiao Qian Zhao Yan Meng Wei Feng School of Mechanical Engineering Chengdu University Chongqing institute of Metrology and Quality Inspection institute of New energy and low-carbon Technology Sichuan University

Oxygen release and electrolyte decomposition under high voltage endlessly exacerbate interfacial ramifications and structu ral degradation of high energy-density Li-rich layered oxide（LLO）,leading to voltage and capacity ***,the dual-strategy of Cr,B complex coating and local gradient doping is simultaneously achieved on LLO surface by a one-step wet chemical reaction at room *** functional theory（DFT） calculations prove that stable B-O and Cr-O bonds through the local gradient doping can significantly reduce the high-energy O 2p states of interfacial lattice O,which is also effective for the near-surface lattice O,thus greatly stabilizing the LLO surface,Besides,differential electrochemical mass spectrometry（DEMS） indicates that the CrxB complex coating can adequately inhibit oxygen release and prevents the migration or dissolution of transition metal ions,including allowing speedy Li+migration,The voltage and capacity fading of the modified cathode（LLO-CrB） are adequately suppressed,which are benefited from the uniformly dense cathode electrolyte interface（CEI） composed of balanced organic/inorganic ***,the specific capacity of LLO-CrB after 200 cycles at 1C is 209.3 mA h g-1（with a retention rate of 95.1%）.This dual-strategy through a one-step wet chemical reaction is expected to be applied in the design and development of other anionic redox cathode materials.

关键词： Interfacial oxygen Lithium-rich layered oxide cathode Local gradient doping One-step wet chemical reaction Surface coating

Pyrrolic nitrogen coordinated Ni^(2+) dual-atom catalyst for boosting CO_(2) electroreduction

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Science China Chemistry 2025年第2期68卷 570-579页

作者： Zhi-Wei Chen Hong-Juan Wang Chang Liu Xiu-Li Lu Tong-Bu Lu MOE International Joint Laboratory of Materials Microstructure Institute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China

Nitrogen-doped carbon materials have been widely used for the constructions of single-atom catalysts,while the effect of different species of doped nitrogen on the catalytic activity of CO_(2) electroreduction has rarely been *** we found that pyrrolic-N coordinated Ni2+catalysts display much higher electrocatalytic CO_(2)-to-CO activity and selectivity than the corresponding pyridinic-N coordinated low valent Ni^((0–+2))catalysts,and pyrrolic-N coordinated Ni2 dual-atoms catalyst of Ni2/N-CNTs exhibits the best electrocatalytic performance,with over 90%Faradaic efficiencies in a broad potentials from−0.6 to−1.2 V *** hydrogen electrode,as well as an outstanding CO specific current of 56.2 A/mgNi and high turnover frequency of 6.2×10^(4) h^(−1),over 7-times higher than those of pyridinic-N coordinated Ni *** results indicate the weak electron-donor nature of pyrrolic-N facilitates the generation of a reduced active site at low overpotential for boosting CO_(2) *** functional theory calculations reveal that the reaction free energy for the*COOH formation on pyrrolic-N coordinated Ni catalysts are lower than those on pyridinic-N coordinated Ni catalysts,and a H_(2)Oadsorbed Ni_(2)/N-CNTs displays the optimized reaction free energy for both*COOH formation and CO desorption,which derive the best catalytic performance.

关键词： dual-atom catalyst CO_(2) electroreduction synergistic catalysis pyrrolic-N pyridinic-N

Metal-organic frameworks with dinuclear metal centers for synergistically boosting CO_(2) photoreduction

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Science China Chemistry 2025年第1期68卷 201-208页

作者： Hui-Feng Wang Wen-Jie Shi Yu-Xin Yang Bao-Xia Dong Tong-Bu Lu Di-Chang Zhong School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China institute for New energy Materials and low carbon Technologies School of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China

Dinuclear metal synergistic catalysis(DMSC)has been proved powerful in boosting CO_(2)reduction,while this has not been achieved in heterogeneous catalysts with long-range order *** this study,we,by introduction of metal catalytic centers into an indium-based metal-organic framework(MOF),obtained a series of isostructural In-MOFs,including three MOFs with mononuclear metal catalytic center(M-In),three MOFs with dinuclear homometallic catalytic centers(MM-In),and three MOFs with dinuclear heterometallic catalytic centers(MM’-In,M/M’=Co(II),Ni(II),Zn(II)).It was found that all these MOFs can serve as catalysts for photochemical CO_(2)reduction to *** with M-In,the catalytic activities of MM-In were obviously enhanced,and that of MM’-In was further significantly *** example,the CO yield of Co Zn-In reaches a record value of 12,700μmol g^(-1)h^(-1),which is 4.0,8.1,9.4,and 18.6-fold higher than that of Co Co-In,Zn Zn-In,Co-In,and Zn-In,***,the catalytic activities of Co Ni-In and Ni Zn-In also show different fold increase than those of corresponding dinuclear homometallic and mononuclear metallic *** results of control experiments and theoretical calculation reveal that the higher catalytic activities of MM-In over M-In can be ascribed to the DMSC effect,and the higher catalytic activity of MM’-In over MM-In can be ascribed to the strengthened DMSC *** work reveals the relationship between DMSC effect and bimetal centers in CO_(2)reduction,which provides new insights into the DMSC and paves a new way to design highly active catalysts for photochemical CO_(2)reduction.

关键词： metal-organic frameworks dinuclear metal centers synergistic catalysis CO_(2)reduction photocatalysis

Unveiling the promotion role of ZnO on Zn-Al spinel oxide for CO_(2)hydrogenation

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Journal of energy Chemistry 2025年第1期100卷 18-25页

作者： Tongyao Wang Xinlong Yao Lixin Liang Hongyu Chen Pan Gao Guangjin Hou State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

The Zn-Al spinel oxide stands out as one of the most active catalysts for high-temperature methanol synthesis from CO_(2)***,the structure–activity relationship of the reaction remains poorly understood due to challenges in atomic-level structural characterizations and analysis of reaction *** this study,we prepared two Zn-Al spinel oxide catalysts via coprecipitation(ZnAl-C)and hydrothermal(ZnAl-H)methods,and conducted a comparative investigation in the CO_(2)hydrogenation ***,under similar conditions,ZnAl-C exhibited significantly higher selectivity towards methanol and DME compared to *** characterizations using X-ray diffraction(XRD),Raman spectroscopy and electron paramagnetic resonance(EPR)unveiled that ZnAl-C catalyst had abundant ZnO species on its surface,and the interaction between the ZnO species and its ZnAl spinel oxide matrix led to the formation of oxygen vacancies,which are crucial for CO_(2)adsorption and ***,state-of-the-art solid-state nuclear magnetic resonance(NMR)techniques,including ex-situ and in-situ NMR analyses,confirmed that the surface ZnO facilitates the formation of unique highly reactive interfacial formate species,which was readily hydrogenated to methanol and *** insights elucidate the promotion effects of ZnO on the ZnAl spinel oxide in regulating active sites and reactive intermediates for CO_(2)-to-methanol hydrogenation reaction,which is further evidenced by the significant enhancement in methanol and DME selectivity observed upon loading ZnO onto the ZnAl-H *** molecular-level mechanism understandings reinforce the idea of optimizing the ZnO-ZnAl interface through tailored synthesis methods to achieve activity-selectivity balance.

关键词： CO_(2)hydrogenation Spinel oxide Zno Solid-state NMR

Synergistic promotion strategy of “dual-site” and “dual-path” to enhance the C–C coupling between CO_(2) 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 ChemistryChinese Academy of ScienceTaiyuan 030001ShanxiChina University of Chinese Academy of Science Beijing 100049China Shenyang University of Chemical Technology Shenyang 110142LiaoningChina

Photoelectrocatalytic coupling CO_(2)and 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 CO_(2)and the competitive hydrogen evolution of ***,a modified g-C_(3)N_(4)/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 g^(-1)h^(-1).As revealed by in-situ characterizations and density functional theory calculations,CO_(2)and HCHO were absorbed at Zn site and N site,***,*CO generated from CO_(2)and HCHO was converted to*CH_(3)O and*CHO on the dual-active-site *** detailed reaction mechanism experiments indicated that C–C coupling only occurred between*CO and*CH_(3)O in electrocatalysis *** from the“*CO+*CH_(3)O”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 CO_(2)and HCHO simultaneously driven by light and electricity.

关键词： g-C_(3)N_(4)/ZnAl-LDH heterojunction Z-scheme C-C coupling Ethanol

Effect of SiO_(2) Nanoparticles/Silicate on Characteristics of Micro-arc Oxidation Coating Formed on TC4 Alloy

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稀有金属材料与工程 2025年第1期54卷 76-83页

作者： Sun Fengyu Yang Zhao Hu Jie Gong Yunbai Wang Ping Luo Qiming Zhu Manlan School of New energy and Materials Southwest Petroleum UniversityChengdu 610500China State Key Laboratory of low-carbon Smart Coal-fired Power Generation and Ultra-clean Emission Nanjing 210046China

TC4 micro-arc oxidation(MAO)coatings were prepared by adding SiO_(2) nanoparticles or sodium silicate to the sodium meta-aluminate-based *** effect of additives was investigated by XRD,SEM,EDS,electrochemical and wear *** results show that additives can considerably accelerate the formation of MAO *** coatings are mostly composed of rutile and anatase TiO_(2),α-Al_(2)O_(3),γ-Al_(2)O_(3),Al_(2)TiO_(5) and SiO_(2).Sodium silicate and SiO_(2) nanoparticles added to the coating can effectively reduce the size of micropores and increase its thickness,whereas SiO_(2) nanoparticles with superior physical properties can be directly deposited at the discharge channel,significantly increasing the coating's resistance to wear and *** coating with SiO_(2) nanoparticles exhibits the best overall performance,with the lowest corrosion rate and average friction coefficient of 4.095×10^(-5)mm/a and 0.30,respectively.

关键词： micro-arc oxidation TC4 alloy coatings corrosion wea

Selenate oxyanion-intercalated NiFeOOH for stable water oxidation via lattice oxygen oxidation mechanism

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Journal of energy Chemistry 2025年第2期101卷 676-684页

作者： Yijie Zhang Weiyi Zhang Xiaowen Zhang Jinping Li Guang Liu Shanxi Key Laboratory of Gas energy Efficient and clean Utilization College of Chemical Engineering and Technology Taiyuan University of Technology Shanxi Research institute of Huai Rou Laboratory

Transition metal-based compounds can serve as pre-catalysts to obtain genuine oxygen evolution reaction（OER） electrocatalysts in the form of oxyhydroxides through electrochemical ***,the role and existence form of leached oxygen anions are still ***,we selected iron selenite-wrapped hydrated nickel molybdate（denoted as NiMoO/FeSeO） as a pre-catalyst to study the oxyanion *** is surprising to find that SeO2-exists in the catalyst in the form of intercalation,which is different from previous studies that suggest that anions are doped with residual elements after electrochemical activation,or adsorbed on the catalyst *** experiment and theoretical calculations show that the existence of SeO42-intercalation effectively adjusts the electronic structure of NiFeOOH,promotes intramolecular electron transfer and O-O release,and thus lowers the reaction energy *** expected,the synthesized NiFeOOH-SeO only needs 202 and 285 mV to attain 100 and 1000 mA cm-2in 1 M ***,the anion exchange membrane water electrolyzer（AEMWE） consisting of NiFeOOHSeO anode and Pt/C cathode can reach 1 A cm-2at 1.70 V and no significant attenuation within 300 *** findings provide insights into the mechanism,by which the intercalated oxyanions enhance the OER performance of NiFeOOH,thereby facilitating large-scale hydrogen production through AEMWE.

关键词： Anion exchange membrane electrolyzer Industrial current densities Lattice oxygen oxidation Oxyanion intercalation Water splitting

Unveiling solid-solid contact states in all-solid-state lithium batteries:An electrochemical impedance spectroscopy viewpoint

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Journal of energy Chemistry 2025年第2期101卷 16-22页

作者： Jin-Liang Li Liang Shen Zi-Ning Cheng Jun-Dong Zhang Ling-Xuan Li Yu-Tong Zhang Yan-Bin Gao Chunli Guo Xiang Chen Chen-Zi Zhao Rui Zhang Qiang Zhang Tsinghua Center for Green Chemical Engineering Electrification Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical Engineering Tsinghua University College of Materials Science and Engineering Taiyuan University of Technology Advanced Research institute of Multidisciplinary Science School of Materials Science and Engineering Beijing Institute of Technology Beijing Huairou Laboratory institute for carbon Neutrality Tsinghua University Shanxi Research institute for clean energy Tsinghua University

All-solid-state lithium batteries（ASSLBs） are strongly considered as the next-generation energy storage devices for their high energy density and intrinsic *** solid-solid contact between lithium metal and solid electrolyte plays a vital role in the performance of working ASSLBs,which is challenging to investigate quantitatively by experimental *** work proposed a quantitative model based on the finite element method for electrochemical impedance spectroscopy simulation of different solid-solid contact states in *** the assistance of an equivalent circuit model and distribution of relaxation times,it is discovered that as the number of voids and the sharpness of cracks increase,the contact resistance Rcgrows and ultimately dominates the battery *** accurate fitting,inverse proportional relations between contact resistance Rcand（1-porosity） as well as crack angle was *** contribution affords a fresh insight into clarifying solid-solid contact states in ASSLBs.

关键词： All-solid-state lithium batteries Distribution of relaxation times Electrochemical impedance spectroscopy Equivalent circuit model Finite element method Solid-solid contacts

Experimental Study on energy Storage Characteristics of Sintered Ore Particle Packed Beds

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Journal of Thermal Science 2025年第1期34卷 242-253页

作者： LAI Zhenya DING Liwei LYU Hongkun HOU Chenglong CHEN Jiaying GUOXutao HAN Gaoyan ZHANG Kang State Grid Zhejiang Electric Power Research institute Hangzhou 310014China State Key Laboratory of clean energy Utilization Zhejiang UniversityHangzhou 310027China

The particle packed bed energy storage system has advantages such as low costs and wide temperature ranges,which can be combined with solar thermal power generation systems to solve the inherent volatility and discontinuity of renewable *** new materials with low costs and excellent storage performances is one of the eternal research hotspots in the field of energy *** paper innovatively uses sintered ore particles as energy storage material and studies the effect of particle size on the airflow resistance characteristics,energy storage characteristics,and thermocline evolution characteristics of the packed bed through thermal energy storage *** results indicate that for the particles in the macro scale,the smaller the particle,the lower the absolute permeability of the bed and the greater the airflow *** packed bed with smaller particles has a larger specific surface area,larger bulk mass,and smaller bed ***,the packed beds with smaller particles have better thermocline characteristics,less irreversible loss,and can achieve higher thermal efficiency and higher exergy efficiency in the heat storage *** cycle thermal efficiency in packed beds with 25-40 mm,16-25 mm,and 10-16 mm particles is 53.58%,56.27%,and 57.60%,respectively,and the cycle exergy efficiency is 61.81%,69.25%,and 74.13%,***,this paper also studies the effect of discharging airflow rates on thermal storage *** experimental results indicate that suitable discharging strategies should be selected based on different heat demands.

关键词： particle packed bed airflow resistance thermal energy storage thermocline evolution