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Catalytic effect in lithium metal batteries: From heterogeneous catalyst to homogenous catalyst

Journal of Energy Chemistry 2024年第3期90卷 305-326,I0008页

作者： Haining Fan Xuan-Wen Gao Hailong Xu Yichun Ding Shi-Xue Dou Wen-Bin Luo School of Fashion and Textiles The Hong Kong Polytechnic UniversityHong Kong 100872China Institute for Energy Electrochemistry and Urban Mines Metallurgy School of MetallurgyNortheastern UniversityShenyang 110819LiaoningChina Institute of Energy Materials Science University of Shanghai for Science and TechnologyShanghai 200000China State Key Laboratory of Solidification Processing School of Materials Science and EngineeringNorthwestern Polytechnical UniversityXi'an 710000ShaanxiChina

Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.

关键词： Energy storage and conversion Metal battery Sulfur battery Air battery Catalytic effect heterogeneous catalyst Homogeneous catalyst

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Enabling heterogeneous catalysis to achieve carbon neutrality: Directional catalytic conversion of CO_(2) into carboxylic acids

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Carbon Energy 2024年第3期6卷 1-35页

作者： Xiaofei Zhang Wenhuan Huang Le Yu Max García-Melchor Dingsheng Wang Linjie Zhi Huabin Zhang KAUST Catalysis Center(KCC) King Abdullah University of Science and Technology(KAUST)ThuwalSaudi Arabia Key Laboratory of Chemical Additives for China National Light Industry College of Chemistry and Chemical EngineeringShaanxi University of Science and TechnologyXi'anChina State Key Lab of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijingChina School of Chemistry CRANN and AMBERResearch CentresTrinity College DublinCollege GreenDublinIreland Department of Chemistry Tsinghua UniversityBeijingChina Advanced Chemical Engineering and Energy Materials Research Center China University of Petroleum(East China)QingdaoChina

The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.

关键词： carbon neutrality carboxylic acids CO_(2)conversion heterogeneous catalyst in situ technology

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A new perspective on hydrogenation of CO2 into methanol over heterogeneous catalysts

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Progress in Natural Science:Materials International 2024年第3期34卷 482-494页

作者： Xueyuan Pan Jingcheng Xu Yali Wang Mingzhe Ma Haiquan Liao Hao Sun Mengmeng Fan Kui Wang Kang Sun Jianchun Jiang Key Lab.of Biomass Energy and Material Jiangsu Province Key and Open Lab.of Forest Chemical Engineering SFA National Engineering Lab.for Biomass Chemical Utilization Institute of Chemical Industry of Forest Products Chinese Academy of Forestry Co-Innovation Center of Efficient Processing and Utilization of Forest Resources Nanjing Forestry University

The utilization of carbon dioxide is critical to realize the objective of "carbon peak and neutrality". Among various carbon dioxide exploitation approaches, catalytic hydrogenation of carbon dioxide is a significant method to selectively convert the CO2into methanol and other valuable chemicals. Among these products, methanol is a crucial chemical feedstock that can be utilized as a platform molecule for the synthesis of chemicals and fuels as well as a fuel for internal combustion engines and fuel cells, causing particular interest. Nowadays, Catalytic hydrogenation of carbon dioxide into methanol has shifted its focus on the creation of low-cost, environmentally friendly, and efficient catalysts. Inspired of this, we have concluded the mechanism of catalytic hydrogenation of carbon dioxide, and reviewed the research progress of multiple heterogeneous catalysts with high catalytic application prospect, especially the supported catalysts.

关键词： Carbon dioxide heterogeneous catalyst Hydrogenation Methanol

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Four unprecedented V_(14)clusters as highly efficient heterogeneous catalyst for CO_(2)fixation with epoxides and oxidation of sulfides

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Science China Chemistry 2023年第1期66卷 107-116页

作者： Ji-Lei Wang Jia-Peng Cao Yin-Hua Zhu Qin Wang Ning-Fang Li Xin-Rong Fan Hua Mei Yan Xu State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing210009China State Key Laboratory of Coordination Chemistry Coordination Chemistry InstituteNanjing UniversityNanjing 210093China

Chemical fixation of carbon dioxide(CO_(2))is an energy-saving method for alleviating the greenhouse gas emissions,whereas it persists a challenge posed by the demand for efficient catalysts.Herein,four unprecedented examples of tetradecanuclear vanadium clusters,namely,[(C_(2)H_(8)N_(2))6(CH_(3)O)8(CH_(3)OH)_(2)V_(10)^(Ⅳ)V_(4)ⅤO_(26)](V_(14)-1),[(C_(3)H_(10)N_(2))_(6)(CH_(3)O)_(8)(CH_(3)OH)_(2)V_(10)^(Ⅳ)V_(4)ⅤO_(26)](V14^(-2)),[(C_(6)H_(14)N_(2))6(CH_(3)O)8(CH_(3)OH)_(2)V_(10)^(Ⅳ)V_(4)ⅤO_(26)]·5H_(2)O(V14^(-3))and[(C_(4)H_(12)N_(2)O)_(4)(C_(4)H_(11)N_(2)O)_(2)(CH_(3)O)_(2)V_(10)^(Ⅳ)V_(4)ⅤO_(28)]·6H_(2)O(V_(14)-4),have been triumphantly designed and constructed under solvothermal conditions.Among them,compounds V_(14)-1–4 are the first cases of tetradecanuclear vanadium clusters without the introduction of inorganic acid radical ions.Two main units[V_(10)^(Ⅳ)V_(4)ⅤO_(26)]8+and[V10ⅣV4ⅤO28]4+represent brand-new configurations of tetradecanuclear vanadium clusters.Given the fact that the presence of V^(Ⅳ)/V^(Ⅴ)can potentially facilitate electron transfer and consequently expedite catalytic reactions,we explored the catalytic activities of these compounds.Remarkably,V_(14)-1 was further used as a heterogeneous catalyst in the CO_(2)fixation into cyclic carbonates under milder conditions(60℃,0.5 MPa)and exhibited higher catalytic activity.Also,the experimental results indicated that V_(14)-1 could efficiently catalyze the sulfoxidation,which could fully convert most sulfides within 40 min at room temperature.Moreover,as a stable heterogeneous catalyst employed in CO_(2)fixation with epoxides and oxidation of sulfides,V_(14)-1 could be consecutively used multiple cycles without losing its catalytic activity.

关键词： V_(14)clusters heterogeneous catalyst CO_(2)fixation oxidation of sulfides

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A natural manganese ore as a heterogeneous catalyst to effectively activate peroxymonosulfate to oxidize organic pollutants

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Chinese Chemical Letters 2022年第11期33卷 4792-4797页

作者： Jinchuan Gu Ping Yin Yi Chen Honglin Zhu Rui Wang School of Food and Bioengineering Civil Engineering and Architecture and EnvironmentEmergency ScienceXihua UniversityChengdu 610039China Sichuan Rongxinkai Engineering Design Co. Ltd.Chengdu 610039China Faculty of Geosciences and Environmental Engineering Southwest Jiaotong UniversityChengdu 611756China

heterogeneous transition metal catalysts are indispensable in improving environmental pollution.However,their fabrication is often costly and cumbersome,and they can easily pollute the environment.This study proposed using a natural Gabonese ore(GBO)containing Mn_(x)O_(y) and FexOy as catalysts to degrade orange Ⅱ(OII)via peroxymonosulfate(PMS)activation.The GBO+PMS system exhibited extraordinarily high stability and catalytic activity towards OII elimination(92.2%,0.0453 min^(−1)).The reactive oxygen species(ROS)generated in the system were identified using radical scavenging tests and electron spin-resonance(ESR)analysis.Singlet oxygen(^(1)O_(2))represented the dominant reactive species for OII degradation,while the system presented a lower reaction energy barrier and was effective in a broad pH range(2-10).This work also proposed the activation mechanism for the GBO+PMS system and OII degradation pathways.This study revealed a new approach for exploring inexpensive,eco-friendly,efficient,and stable heterogeneous transition metal catalysts.

关键词： Transition metal heterogeneous catalyst Natural ore OrangeⅡ Peroxymonosulfate

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Differentially-grown cobalt regulators cooperatively involved in the tandem catalysis for high-yield production of second amines

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Nano Research 2024年第4期17卷 2444-2450页

作者： Jinhui Xu Xiao Wang Ying Wang Fei Wang Lingling Zhang Wenjie Cui Shuyan Song Hongjie Zhang State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China Department of Chemistry Tsinghua UniversityBeijing 100084China

One-pot tandem catalysis has been regarded as one of the most atomic economic ways to produce secondary amines,the important platform molecules for chemical synthesis and pharmaceutical manufacture,but it is facing serious issues in overall efficiency.New promotional effects are highly desired for boosting the activity and regulating the selectivity of conventional tandem catalysts.In this work,we report a high-performance tandem catalyst with maximized synergistic effect among each counterpart by preciously manipulating the spatial structure,which involves the active CeO_(2)/Pt component as kernel,the densely-coated N-doped C(NC)layer as selectivity controller,and the differentially-grown Co species as catalytic performance regulators.Through comprehensive investigations,the unique growth mechanism and the promotion effect of Co regulators are clarified.Specifically,the surface-landed Co clusters(Cocs)are crucial to selectivity by altering the adsorption configuration of benzylideneaniline intermediates.Meanwhile,the inner Co particles(Cops)are essential for activity by denoting their electrons to neighboring Ptps.Benefiting from the unique promotion effect,a remarkably-improved catalytic efficiency(100%nitrobenzene conversion with 94%N-benzylaniline selectivity)is achieved at a relatively low temperature of 80℃,which is much better than that of CeO_(2)/Pt(100%nitrobenzene conversion with 12%N-benzylaniline selectivity)and CeO_(2)/Pt/NC(35%nitrobenzene conversion with 94%benzylideneaniline selectivity).

关键词： tandem catalysis CeO_(2) hierarchical structure heterogeneous catalyst dual-site materials

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Selective photosynthesis of imines from biomass-derived aldehydes over Ni/TiO_(2)

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Rare Metals 2024年第3期43卷 1116-1124页

作者： Wu-Lin Li Qing-Qing Zhang Lin Dong Wen-Jun Zhang Li-Li Lin Zu-Peng Chen Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources International Innovation Center for Forest Chemicals and MaterialsCollege of Chemical EngineeringNanjing Forestry UniversityNanjing210037China Institute of Industrial Catalysis State Key Laboratory of Green Chemistry Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou310014China

Photocatalytic reductive amination of biomass-derived aldehydes is a desirable way to selectively upgrade biomass into value-added nitrogen-containing chemicals under mild conditions.However,it is challenging to produce imines in high selectivity because of the undesirable side reactions caused by the activity of functional groups.Here,we demonstrate the highly reactive and selective production of imines from biomass derived aldehydes via the photocatalytic reductive amination,using a defective TiO_(2)supported nickel catalyst.The employment of methanol as the hydrogen donor and ammonia solution as the nitrogen source avoids the use of high-pressure H_(2)and expensive amines,rendering the current catalytic process safe,economical,and environmentally friendly.In depth investigations attribute the improved separation and transfer of photogenerated charge carriers to the presence of oxygen vacancies and decorated Ni nanoparticles,thereby accelerating the production of imines from benzaldehyde amination(conversion,95.8%;seleetivity,95.2%).Furthermore,the developed system could be easily translated to the photocatalytic conversions of various biomass derived aldehydes,which provided an example of a cost-effective and sustainable approach for the valorization of biomass derived feedstocks.

关键词： Photocatalysis Biomass derivatives Imines Reduction amination heterogeneous catalyst

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Activity promotion of Rh_(1)Ca_(x)/Al_(2)O_(3) single-atom catalyst in 1-octene hydroformylation:a volcano curve exists between Ca adding ratio and catalytic activity

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Science China Chemistry 2024年第4期67卷 1187-1192页

作者： Hao Zhang Xingcong Zhang Xilun Wang Qingdi Sun Hao Liu Hongbing Ji Xiaohui He Key Laboratory of Bioinorganic and Synthetic Chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou 510275China Huizhou Research Institute Sun Yat-sen UniversityHuizhou 516081China State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China

Single-atom catalysts(SACs)are considered the best candidates for olefin hydroformylation due to their combined advantages of homogeneous and heterogeneous catalysts.Unlike conventional organo-phosphine modification,Rh SAC is modified by introducing Ca,resulting in a significant increase in activity(maximum~5.7-fold)and stability.Furthermore,a volcano curve between Ca addition ratio and catalytic activity is found.Introducing Ca significantly increases activity by decreasing the energy barrier,but excessive Ca decreases activity due to hindering substrate adsorption and reaction.

关键词： hydroformylation bimetallic single-atom catalysts rhodium heterogeneous catalyst

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Oxide-supported metal catalysts for anaerobic NAD+regeneration with concurrent hydrogen production

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Chinese Chemical Letters 2024年第2期35卷 263-267页

作者： Jianwei Li Joseph W.H.Burnett Claudia Martinez Macias Russell F.Howe Xiaodong Wang Chemical Engineering School of EngineeringLancaster UniversityLancaster LA1 4YWUnited Kingdom Chemistry Department University of AberdeenAberdeen AB24 3UEUnited Kingdom

We report SiO_(2)-supported monometallic Pt,Pd,Au,Ni,Cu and Co catalysts for proton-driven NAD+regeneration,co-producing H_(2).All metals are fully selective to NAD+where the order of turnover frequencies(Pt>Pd>Cu>Au,Ni and Co)coincides with those otherwise observed in electrochemical hydrogen evolution reactions.This has revealed that NADH is capable of converting the metal sites into a“cathode”without an external potential and the NADH to NAD+reaction involves transferring electron and hydrogen atom separately.Electron-deficient Ptδ+(on CeO_(2))enhances TOF and the heterogeneous Pt/CeO_(2) catalyst is recyclable without losing any activity/selectivity.

关键词： NAD+regeneration heterogeneous catalyst Hydrogenase mimic Hydrogen binding energy Hydrogen production

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Solar-Driven Hydrogen Peroxide Production Using Polymer-Supported Carbon Dots as heterogeneous catalyst

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Nano-Micro Letters 2017年第4期9卷 30-40页

作者： Satyabrat Gogoi Niranjan Karak Advanced Polymer and Nanomaterial Laboratory Department of Chemical SciencesTezpur UniversityTezpur 784028AssamIndia

Safe, sustainable, and green production of hydro gen peroxide is an exciting proposition due to the role of hydrogen peroxide as a green oxidant and energy carrier for fuel cells. The current work reports the development of carbon dot-impregnated waterborne hyperbranched polyurethane as a heterogeneous photo-catalyst for solar-driven production of hydrogen peroxide. The results reveal that the carbon dots possess a suitable band-gap of 2.98 eV,which facilitates effective splitting of both water and ethanol under solar irradiation. Inclusion of the carbon dots within the eco-friendly polymeric material ensures their catalytic activity and also provides a facile route for easy catalyst separation, especially from a solubilizing medium.The overall process was performed in accordance with the principles of green chemistry using bio-based precursorsand aqueous medium. This work highlights the potential of carbon dots as an effective photo-catalyst.

关键词： Carbon dot Photo-catalyst heterogeneous catalyst Hydrogen peroxide

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