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Diatomic Pd catalyst with conjugated backbone for synergistic electrochemical CO_(2)reduction

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Nano Research 2024年第6期17卷 4850-4855页

作者： Wenxuan Zhang Mengran Zhang Hongjuan Wang Wen Zhang Min Zhang 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 Tianjin Key Laboratory of Organic Solar Cells and Photochemical Conversion School of Chemistry and Chemical EngineeringTianjin University of TechnologyTianjin 300384China

Double-site catalysts have attracted widespread attention in the field of electrocatalysis due to their high metal loading,adjustable active centres,and electronic valence ***,the development of bimetallic sites catalysts that coordinate with definite atoms is still in the exploratory ***,we designed and synthesized a bimetallic palladium complex(BPB-Pd_(2))with conjugated *** supported BPB-Pd_(2)was applied to electrochemical CO_(2)reduction reaction(CO_(2)RR)for the first *** as-obtained BPB-Pd_(2)gives an exceptional Faradaic efficiency of CO(FECO)of 94.4%at−0.80 V *** hydrogen electrode(RHE),which is significantly superior to monoatomic palladium catalyst(BPB-Pd1).The density functional theory(DFT)calculations revealed that the essential reason for the outstanding activity of BPB-Pd_(2)toward CO_(2)RR was that the electronic effect between diatomic palladium reduces the free energy change for CO_(2)RR ***,BPB-Pd_(2)exhibits moderate free energy change to form COOH*intermediate,which was beneficial for the generation of CO in CO_(2)RR.

关键词： synthesis electrocatalysis CO_(2)reduction bimetallic palladium complex synergistic catalysis

Nickel-modified In_(2)O_(3) with inherent oxygen vacancies for CO_(2) hydrogenation to methanol

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Science China Chemistry 2024年第5期67卷 1715-1728页

作者： Zixuan Zhou Yuchen Wang Yuanjie Bao Haiyan Yang Jiong Li Chunran Chang Shenggang Li Peng Gao CAS Key Laboratory of low-carbon Conversion Science and Engineering Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China University of Chinese Academy of Sciences Beijing 100049China School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China Shaanxi Key Laboratory of low Metamorphic Coal Clean Utilization School of Chemistry and Chemical EngineeringYulin UniversityYulin 719000China

Methanol synthesis is one of the most important industrially-viable approaches for carbon dioxide(CO_(2)) utilization, as the produced methanol can be used as a platform chemical for manufacturing green fuels and chemicals. The In_(2)O_(3) catalysts are ideal for sustainable methanol synthesis and have received considerable attention. Herein, Co-, Ni-and Cu-modified In_(2)O_(3) catalysts were fabricated with high dispersion and high stability to improve the hydrogenation performance. The Ni-promoted In_(2)O_(3) catalyst in the form of high dispersion possessed the largest amount of oxygen vacancies and the strongest ability for H_(2) activation, leading to the highest CO_(2) conversion and space time yield of methanol of 0.390 g_(Me OH)g_(cat)^(-1)h^(-1) with CH_(3)OH selectivity of 68.7%. In addition, the catalyst exhibits very stable performance over 120 h on stream, which suggests the promising prospect for industrial applications. Further experimental and theoretical studies demonstrate that surface Ni doping promotes the formation of oxygen defects on the In_(2)O_(3) catalyst, although it also results in lower methanol selectivity. Surprisingly, subsurface Ni dopants are found to be more beneficial for methanol formation than surface Ni dopants, so the Nipromoted In_(2)O_(3)catalyst with a lower surface Ni content at the similar Ni loading can reach higher methanol selectivity and productivity. This work thus provides theoretical guidance for significantly improving the CO_(2) reactivity of In_(2)O_(3)-based catalysts while maintaining high methanol selectivity.

关键词： carbon dioxide hydrogenation methanol synthesis indium oxides Ni doping sites transition metal promoters

Building Fe atom–cluster composite sites using a site occupation strategy to boost electrochemical oxygen reduction

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carbon Energy 2024年第3期6卷 276-286页

作者： Tingyi Zhou Yi Guan Changjie He Lei Zhang Xueliang Sun Zhongxin Song Qianling Zhang Chuanxin He Xiantao Jiang Zhaoyan Luo Wei Xing Xiangzhong Ren College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdongChina Department of Mechanical and Materials Engineering University of Western OntarioLondonOntarioCanada State Key Laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesJilinChangchunChina

The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic clusters to ***,understanding the interactions among these components,especially the synergistic effects between single atomic sites and cluster sites,is crucial for improving the oxygen reduction reaction(ORR)activity of M–N–C ***,herein,we constructed a model catalyst composed of both atomically dispersed FeN4 SA sites and adjacent Fe clusters through a site occupation *** found that the Fe clusters can optimize the adsorption strength of oxygen reduction intermediates on FeN4 SA sites by introducing electron-withdrawing–OH ligands and decreasing the d-band center of the Fe *** as-developed catalyst exhibits encouraging ORR activity with halfwave potentials(E1/2)of 0.831 and 0.905 V in acidic and alkaline media,***,the catalyst also represents excellent durability exceeding that of Fe–N–C SA *** practical application of Fe(Cd)–CNx catalyst is further validated by its superior activity and stability in a metalair battery *** work exhibits the great potential of synergistic effects between multiphase metal species for improvements of singleatom site catalysts.

关键词： d-band center metal clusters oxygen reduction reaction single-atom catalyst site occupations strategy

Sono-photocatalytic amination of quinoxalin-2(1H)-ones with aliphatic amines

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Chinese Chemical Letters 2024年第10期35卷 269-272页

作者： Wen-Tao Ouyang Jun Jiang Yan-Fang Jiang Ting Li Yuan-Yuan Liu Hong-Tao Ji Li-Juan Ou Wei-Min He School of Chemistry and Chemical Engineering University of South ChinaHengyang 421001China School of Materials Science and Engineering Hunan Institute of TechnologyHengyang 421002China National Engineering Research Center of low-carbon Processing and Utilization of Forest Biomass Nanjing Forestry UniversityNanjing 210037China

The first example of sono-photocatalytic bond formation was *** both visible light and ultrasound wave as the energy,various 3-aminoquinoxalin-2(1H)-ones were efficiently obtained with good functional group tolerance in the absence of any additive or external *** with the conventional photocatalysis,sono-photocatalysis not only dramatically improved the reaction rates and yields,but also reduced energy consumption.

关键词： Sono-photocatalysis External photocatalyst-free Quinoxalin-2(1H)-ones Amination Aliphatic amines

Evolution of pore systems in low-maturity oil shales during thermal upgrading--Quantified by dynamic SEM and machine learning

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Petroleum Science 2024年第3期21卷 1739-1750页

作者： Jun Liu Xue Bai Derek Elsworth Key Laboratory of Deep Underground Science and Engineering(Ministry of Education) Institute of New Energy and Low-Carbon TechnologySichuan UniversityChengdu610065SichuanChina International Quantum Academy Shenzhen518048GuangdongChina Shenzhen institute of Advanced Electronic Materials Shenzhen Institute of Advanced TechnologyChinese Academy of SciencesShenzhen518055GuangdongChina Department of Energy and Mineral Engineering Pennsylvania State University ParkPA 16802USA

In-situ upgrading by heating is feasible for low-maturity shale oil,where the pore space dynamically *** characterize this response for a heated substrate concurrently imaged by *** systematically follow the evolution of pore quantity,size(length,width and cross-sectional area),orientation,shape(aspect ratio,roundness and solidity)and their anisotropy—interpreted by machine *** indicate that heating generates new pores in both organic matter and inorganic ***,the newly formed pores are smaller than the original pores and thus reduce average lengths and widths of the bedding-parallel pore ***,the average pore lengths and widths are increased in the bedding-perpendicular ***,heating increases the cross-sectional area of pores in low-maturity oil shales,where this growth tendency fluctuates at300℃.In addition,the orientation and shape of the newly-formed heating-induced pores follow the habit of the original pores and follow the initial probability distributions of pore orientation and ***,limited anisotropy is detected in pore direction and shape,indicating similar modes of evolution both bedding-parallel and *** propose a straightforward but robust model to describe evolution of pore system in low-maturity oil shales during heating.

关键词： low-maturity oil shale Pore elongation Organic matter pyrolysis In-situthermal upgrading Scanning electron microscopy(SEM) Machine learning

Comprehensive analysis and mitigation strategies for safety issues of sodium-ion batteries

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Rare Metals 2024年第4期43卷 1343-1349页

作者： Tao Wei Xiao-Ling Xian Shi-Xue Dou Wei Chen Shu-Lei Chou institute for carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou325035China Wenzhou Key Laboratory of Sodium-Ion Batteries Wenzhou University Technology Innovation Institute for Carbon NeutralizationWenzhou325035China Zhejiang Key Laboratory of carbon Materials College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou325035China institute for Superconducting and Electronic Materials Australian Institute for Innovative MaterialsUniversity of WollongongInnovation CampusWollongongNSW2522Australia

Sodium-ion batteries show great potential as an alternative energy storage system,but safety concerns remain a major hurdle to their mass *** paper analyzes the key factors and mechanisms leading to safety issues,including thermal runaway,sodium dendrite,internal short circuits,and gas *** promising solutions are proposed,such as high-safety electrode materials in the cathode and anode,high-safety electrolytes,and external battery management *** in also we emphasize the importance of selecting appropriate analysis methods and developing reliable failure models while suggesting advanced machine learning tools for *** a comprehensive approach,this study offers valuable recommendations to optimize materials and solutions for improving the safety of sodium-ion batteries.

关键词： Sodium-ion batteries Safety issues Thermal runaway Sodium dendrites

Top 10 Influential Events in carbon neutrality and climate change response for 2023

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Frontiers in Energy 2024年第1期18卷 1-3页

作者： Research institute of carbon Neutrality of Shanghai Jiao Tong University Research institute of carbon Neutrality Shanghai Jiao Tong UniversityShanghai 200240China

In 2023, the global community intensified its efforts towards achieving carbon neutrality and addressing climate change, witnessing several impactful events. Research institute of carbon Neutrality, Shanghai Jiao Tong University compiled the Top 10 Events (in chronological order) in the field of global carbon neutrality and climate change response for 2023, to share with readers these significant moments that document the ongoing ambition and collective efforts of human society.

关键词： neutral collective intensified

High-Performance Recyclable Furan-based Epoxy Resin and Its carbon Fiber Composites with Dense Hydrogen Bonding

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Chinese Journal of Polymer Science 2024年第1期42卷 73-86,I0008页

作者： Chang-Bo Zhao Lu-Kun Feng Hui Xie Ming-Liang Wang Bing Guo Zhi-Yong Xue Cai-Zhen Zhu Jian Xu Advanced Materials Research institute North China Electric Power UniversityBejing 102206China institute of low-Dimensional Materials Genome Initiative College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China Chengdu institute of Organic Chemistry Chinese Academy of SciencesChengdu 610041China School of Science and Shenzhen Key Laboratory of Flexible Printed Electronics Technology and Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive ApplicationHarbin Institute of TechnologyShenzhen 518055China

The emerging biomass-based epoxy vitrimers hold great potential to fulfill the requirements for sustainable development of *** the existence of dynamic chemical bonds in vitrimers often reduces both the thermal and mechanical properties of epoxy resins, it is challenging to produce recyclable epoxy vitrimers with both excellent mechanical properties and good thermal stability. Herein, a monomer 4-(((5-(hydroxymethyl)furan-2-yl)methylene)amino)phenol(FCN) containing furan ring with potential to form high density of hydrogen bonding among repeating units is designed and copolymerized with glycerol triglycidyl ether to yield epoxy resin(FCN-GTE), which intrinsically has dual hydrogen bond networks, dynamic imine structure and resultant high performance. Importantly, as compared to the BPA-GTE, the FCN-GTE exhibits significantly improved mechanical properties owing to the increased density of hydrogen bond network and physical crosslinking interaction. Furthermore, density functional theory(DFT) calculation and in situ FTIR analysis is conducted to decipher the formation mechanism of hydrogen bond network. In addition, the FCN-GTE possesses superior UV shielding, chemical degradation, and recyclability because of the existence of abundant imine bonds. Notably, the FCN-GTE-based carbon fiber composites could be completely recycled in an amine *** study provides a facile strategy for synthesizing recyclable biomass-based high-performance epoxy vitrimers and carbon fiber composites.

关键词： Furan Hydrogen bond network Dynamic Schiff base carbon fiber composites Recycling

Suppressing the lattice oxygen diffusion via high-entropy oxide construction towards stabilized acidic water oxidation

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Nano Research 2024年第3期17卷 1107-1113页

作者： Jing Ni Zhaoping Shi Yibo Wang Jiahao Yang Hongxiang Wu Pengbo Wang Kai Li Meiling Xiao Changpeng Liu Wei Xing State Key Laboratory of Electroanalytic Chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The scale-up deployment of ruthenium(Ru)-based oxygen evolution reaction(OER)electrocatalysts in proton exchange membrane water electrolysis(PEMWE)is greatly restricted by the poor *** the lattice-oxygen-mediated mechanism(LOM)has been identified as the major contributor to the fast performance degradation,impeding lattice oxygen diffusion to inhibit lattice oxygen participation is imperative,yet remains challenging due to the lack of efficient ***,we strategically regulate the bonding nature of Ru–O towards suppressed LOM via Ru-based high-entropy oxide(HEO)*** lattice disorder in HEOs is believed to increase migration energy barrier of lattice *** a result,the screened Ti_(23)Nb_(9)Hf_(13)W_(12)Ru_(43)O_(x) exhibits 11.7 times slower lattice oxygen diffusion rate,84%reduction in LOM ratio,and 29 times lifespan extension compared with the state-of-the-art RuO_(2) *** work opens up a feasible avenue to constructing stabilized Ru-based OER catalysts towards scalable application.

关键词： ruthenium-based high-entropy oxide suppressing the lattice oxygen diffusion acidic oxygen evolution reaction