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Novel carbon-nitride based catalysts for enhanced CH_(4) reforming under visible light: From morphology to heterojunction design principles

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能源化学:英文版 2023年第8期83卷 423-432,I0011页

作者： Yufei Huang Ding Wei Ziyi Li Yu Mao Yangqiang Huang Bo Jin Xiao Luo Zhiwu Liang Joint International Center for CO_(2)Capture and Storage(iCCS) The Engineering Research Center of Advanced CatalysisMinistry of Education ProvincialHunan Key Laboratory for Cost-effective Utilization of Fossil Fuel Aimed at Reducing CO_(2)EmissionsCollege of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082HunanChina

The synthesis of high value-added chemical products using CO_(2)and CH_(4)is a promising CO_(2)conversion technology that can reduce greenhouse gas emissions while also alleviating the energy ***,problems such as high energy consumption and strict reaction conditions in reforming process hinder the further development of the *** this work,carbon-nitrogen based composites were prepared for the first time according to the design principle from morphology to heterojunction,which is innovatively applied in the process of photocatalytic ***,C_(3)N_(4)materials with different dimensions(D) are prepared and applied to a CO_(2)-CH_(4)photocatalytic ***,the 2D/2D TiO_(2)/g-C_(3)N_(4)heterostructure is constructed with the ultrasonic impregnation method to further improve charge generation,transfer,and separation *** is worth noting that the yield of CO reaches173.80 μmol g^(-1),and the catalytic performance is improved by 1546% compared to bulk C_(3)N_(4).Moreover,the physical and chemical properties of 2D/2D TiO_(2)/g-C_(3)N_(4)materials are studied using a variety of cha racterization ***,the work fu nction and adsorption energy of different C3N4/TiO_(2)models for CO_(2)adsorption are calculated by density functional theory(DFT).Then,a possible catalytic mechanism for photocatalytic CO_(2)and CH_(4) conversion is proposed based on DFT calculations and experimental *** work provides a new technical route for the rapid conversion of CO_(2)and CH_(4) at room temperature,as well as a new research concept for achieving carbon neutrality.

关键词： Photocatalytic CO_(2) CH_(4) 2D/2DTiO_(2)/g-C_(3)N_(4) Conversion

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Highly efficient multiplex base editing:One-shot deactivation of eight genes in Shewanella oneidensis MR-1

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Synthetic and Systems Biotechnology 2023年第1期8卷 1-10页

作者： Yaru Chen Meijie Cheng Yan Li Lin Wang Lixia Fang Yingxiu Cao Hao Song Frontier Science Center for Synthetic Biology and key laboratory of Systems Bioengineering(ministry of education) School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China key laboratory of Systems Bioengineering(ministry of education) Tianjin UniversityTianjin300072China

Obtaining electroactive microbes capable of efficient extracellular electron transfer is a large undertaking for the scalability of bio-electrochemical ***,researchers need to pursue the co-modification of multiple genes rather than expecting that modification of a single gene would make a significant contribution to improving extracellular electron transfer *** editing has enabled highly-efficient gene deactivation in model electroactive microbe Shewanella oneidensis *** multiplexed application of base editing is still limited by its low throughput procedure,we thus here develop a rapid and efficient multiplex base editing system in *** approaches to express multiple gRNAs were assessed firstly,and transcription of each gRNA cassette into a monocistronic unit was validated as a more favorable option than transcription of multiple gRNAs into a polycistronic ***,a smart scheme was designed to deliver one-pot assembly of multiple gRNAs.3,5,and 8 genes were deactivated using this system with editing efficiency of 83.3%,100%and 12.5%,*** offer some nonrepetitive components as alternatives genetic parts of sgRNA cassette,different promoters,handles,and terminators were *** multiplex base editing tool was finally adopted to simultaneously deactivate eight genes that were identified as significantly downregulated targets in transcriptome analysis of riboflavin-overproducing strain and control *** maximum power density of the multiplex engineered strain HRF(8BE)in microbial fuel cells was 1108.1 mW/m2,which was 21.67 times higher than that of the wild-type *** highly efficient multiplexed base editing tool elevates our ability of genome manipulation and combinatorial engineering in Shewanella,and may provide valuable insights in fundamental and applied research of extracellular electron transfer.

关键词： Multiplex gene editing Electroactive microorganisms Base editing Multiplexed engineering CRISPR Extracellular electron transfer

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燃烧源氨排放对灰霾期间北京大气铵的重要贡献

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Science Bulletin 2024年第7期69卷 978-987页

作者：吴礼彬王芃张强任红 Zongbo Shi 胡伟陈静谢巧蓉李林杰越思瑶韦莲芳宋琳琳张永根王子涵陈爽韦琬王小曼章炎麟孔少飞葛宝珠杨婷方运霆任露洁邓君俊孙业乐王自发张宏亮胡建林刘丛强 Roy M.Harrison Qi Ying 傅平青 Institute of Surface-Earth System Science School of Earth System ScienceTianjin UniversityTianjin 300072China Department of Atmospheric and Oceanic Sciences Fudan UniversityShanghai 200438China IRDR ICoE on Risk Interconnectivity and Governance on Weather/Climate Extremes Impact and Public Health Fudan UniversityShanghai 200438China ministry of education key laboratory for Earth System Modeling Department of Earth System ScienceTsinghua UniversityBeijing 100084China Air Environmental Modeling and Pollution Controlling key laboratory of Sichuan Higher education Institute Chengdu University of Information TechnologyChengdu 610225China Division of Environmental Health&Risk Management School of GeographyEarth&Environmental SciencesUniversity of BirminghamBirmingham B152TTUK School of Environmental Science and Engineering Tianjin UniversityTianjin 300072China State key laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry Institute of Atmospheric PhysicsChinese Academy of SciencesBeijing 100029China key laboratory of Forest Ecology and Management Institute of Applied EcologyChinese Academy of SciencesShenyang 110164China Yale-NUIST Center on Atmospheric Environment International Joint Laboratory on Climate and Environment ChangeNanjing University of Information Science and TechnologyNanjing 210044China Department of Atmospheric Sciences School of Environmental Studies and Department of Environmental Science and TechnologySchool of Environmental StudiesChina University of GeosciencesWuhan 430074China Department of Environmental Science and Engineering Fudan UniversityShanghai 200438China Collaborative Innovation Center of Atmospheric Environment and Equipment Technology Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution ControlNanjing University of Information Science and TechnologyNanjing 210044China Department of Environmental Sciences/Center of Excellence in Environmental Studies King Abdulaziz UniversityJeddah 21589Saudi Arabia Zachr

Aerosol ammonium(NH_(4)^(+)),mainly produced from the reactions of ammonia(NH_(3))with acids in the atmosphere,has significant impacts on air pollution,radiative forcing,and human *** the source and formation mechanism of NH_(4)^(+)can provide scientific insights into air quality ***,the sources of NH_(3)in urban areas are not well understood,and few studies focus on NH_(3)/NH_(4)^(+)at different heights within the atmospheric boundary layer,which hinders a comprehensive understanding of aerosol NH_(4)^(+).In this study,we perform both field observation and modeling studies(the Community Multiscale Air Quality,CMAQ)to investigate regional NH_(3)emission sources and vertically resolved NH_(4)^(+)formation mechanisms during the winter in *** stable nitrogen isotope analyses and CMAQ model suggest that combustion-related NH_(3)emissions,including fossil fuel sources,NH_(3)slip,and biomass burning,are important sources of aerosol NH_(4)^(+)with more than 60%contribution occurring on heavily polluted *** contrast,volatilization-related NH_(3)sources(livestock breeding,N-fertilizer application,and human waste)are dominant on clean ***-related NH_(3)is mostly local from Beijing,and biomass burning is likely an important NH_(3)source(~15%–20%)that was previously *** effective control strategies such as the two-product(e.g.,reducing both SO_(2)and NH_(3))control policy should be considered to improve air quality.

关键词： Particulate ammonium Nitrogen isotope PM2.5 The Community Multiscale Air Quality(CMAQ) Control policy

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The confined growth of few-layered and ultrashort-slab Ni-promoted MoS_(2)on reduced graphene oxide for deep-degree hydrodesulfurization

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Nano Research 2022年第8期15卷 7052-7062页

作者： Dongxu Wang Lei Wang Yanqing Jiao Aiping Wu Haijing Yan Xin Kang Chungui Tian Jiancong Liu Honggang Fu key laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080China

Hydrodesulfurization(HDS)is an essential process in clean fuel oil production,however,the huge challenge is the synthesis of the catalyst with plentiful active ***,we have shown the design of few-layered,ultrashort Ni-Mo-S slabs dispersed on reduced graphene oxide(Ni-Mo-S/rGO-A)based on anchoring[PMo_(12)O_(40)]3−clusters and Ni^(2+)on polyethyleneimine(PEI)-modified graphite *** characterizations(transmission electron microscopy(TEM),X-ray absorption fine structure(XAFS),etc.)show that Ni-Mo-S slabs with predominant monolayer and partial substitution of edge Mo atoms by isolated Ni atoms have rich accessible edge Ni-Mo-S sites and high sulfurization *** virtues endow it with plentiful edge-active sites,and consequently,the enhanced performance for hydrodesulfurization of dibenzothiophene(DBT).The hydrodesulfurization proceeds via a more-favorable direct desulfurization(DDS)route with a reaction rate constant(kHDS)of 48.6×10^(−7)mol·g^(−1)·s^(−1)over Ni-Mo-S/rGO-A catalyst,which is 4.3 times greater than that over traditional Ni-Mo-S/Al_(2)O_(3)catalyst and at the forefront of reported catalysts.

关键词： few-layered Ni-promoted MoS_(2) confined growth reduced graphene oxide high sulfurization degree hydrodesulfurization

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Chemisorption solid materials for hydrogen storage near ambient temperature:A review

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Frontiers in Energy 2023年第1期17卷 72-101页

作者： Yiheng ZHANG Shaofei WU Liwei WANG Xuefeng ZHANG Institute of Refrigeration and Gryogenic Key Laboratory of Power Machinery and Engineering of the Ministry of EducationShanghai Jiao Tong UniversityShanghai 200240China

Solid chemisorption technologies for hydrogen storage,especially high-efficiency hydrogen storage of fuel cells in near ambient temperature zone defined from−20 to 100℃,have a great application potential for realizing the global goal of carbon dioxide emission reduction and vision of carbon ***,there are several challenges to be solved at near ambient temperature,i.e.,unclear hydrogen storage mechanism,low sorption capacity,poor sorption kinetics,and complicated synthetic *** this review,the characteristics and modification methods of chemisorption hydrogen storage materials at near ambient temperature are *** interaction between hydrogen and materials is analyzed,including the microscopic,thermodynamic,and mechanical *** on the classification of hydrogen storage metals,the operation temperature zone and temperature shifting methods are discussed.A series of modification and reprocessing methods are summarized,including preparation,synthesis,simulation,and experimental ***,perspectives on advanced solid chemisorption materials promising for efficient and scalable hydrogen storage systems are provided.

关键词： hydrogen storage capacity chemisorption near-ambient-temperature modification methods alloy hydrides

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Experimental and Modelling Study on Emission of Volatile Nitrogen Derived NO during Pressured Oxy-fuel Combustion under Wet Flue Gas Environment

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Journal of Thermal Science 2023年第5期32卷 1750-1757页

作者： ZAN Haifeng CHEN Xiaoping PAN Suyang GENG Pengfei LIU Daoyin MA Jiliang LIANG Cai key laboratory of Energy Thermal Conversion and Control of ministry of education School of Energy&EnvironmentSoutheast UniversityNanjing 210096China

Pressurised oxy-fuel combustion(POFC)is a clean and efficient combustion technology with great *** to the recycling of flue gas,the concentration of steam in the flue gas is higher than that of conventional combustion,which enriches the free radical pool in the flue gas and thus affects the emission of gaseous ***,further research into the effect of high steam concentrations on NO_(x)emission mechanisms in POFC is *** this work,a fixed-bed reactor was used to conduct combustion experiments of volatiles and combined with chemical kinetic models to study the NO release characteristics for different pressures and steam concentrations in an O_(2)/CO_(2)atmosphere at 800℃/900℃*** results of the study indicated that the volatile nitrogen comes from the pyrolysis of part of pyrrole,pyridine,and all quaternary nitrogen in *** increase in temperature promoted the formation of NO during *** pressure affects the main reaction pathway for NO formation,promoting NO consumption by HCCO and C_(2)O groups while enhancing the overall NO *** promoted NO consumption by *** addition,steam increased the amount of H/OH groups during the reaction,which affected both NO formation and ***,from the overall effect,the steam still inhibits the emission of NO.

关键词： pressurized oxy-fuel combustion steam volatile nitrogen NO emission

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Modeling of Packed Bed Methanol Steam Reformer Integrated with Tubular High Temperature Proton Exchange Membrane fuel Cell

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Journal of Thermal Science 2023年第1期32卷 81-92页

作者： LIU Menghua SHI Yixiang CAI Ningsheng key laboratory for Thermal Science and Power Engineering of ministry of education Department of Energy and Power EngineeringTsinghua UniversityBeijing 100084China

This work proposes a novel tubular structure of high-temperature proton exchange membrane fuel cell(PEMFC)integrated with a built-in packed-bed methanol steam reformer to provide hydrogen for power output.A two-dimensional axisymmetric non-isothermal model was developed in COMSOL Multiphysics 5.4 to simulate the performance of a tubular high temperature proton membrane fuel cell and a packed bed methanol *** model considers the coupling multi-physical processes,including methanol reforming reaction,water gas shift reaction,methanol cracking reaction as well as the heat,mass and momentum transport *** sub-model of the tubular packed-bed methanol reformer is validated between 433 K and 493 K with the experimental data reported in the *** sub-model of the high temperature proton exchange fuel cell is validated between 393 K and 433 K with the published *** results show that power output and temperature distribution of the integrated unit depend on methanol flow rates and working *** was suggested that stable power generation performance of 0.14 W/cm_(2)and temperature drop in methanol steam reformer of≤10 K could be achieved by controlling the methanol space-time ratio of≥250 kg·s/mol with working voltage at 0.6 V,even in the absence of an external heat source.

关键词： high temperature proton exchange membrane fuel cell methanol steam reformer tubular PEMFC hydrogen production Multiphysics modeling

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Synthesis of high density and low freezing point jet fuels range cycloalkanes with cyclopentanone and lignin-derived vanillins

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Journal of Energy Chemistry 2023年第4期79卷 22-30页

作者： Xinghua Zhang Miaojia Song Jianguo Liu Qi Zhang Lungang Chen Longlong Ma key laboratory of Energy Thermal Conversion and Control of ministry of education School of Energy and EnvironmentSoutheast UniversityNanjing 210096JiangsuChina

In this work,a“cyclopentanone-vanillin”strategy was proposed for the preparation of jet fuel range cycloalkanes from lignocellulose-derived ketones and lignin-derived aldehydes via aldol condensation and hydrodeoxygenation(HDO).Ethanolamine lactate ionic liquid(LAIL)exhibited excellent catalytic activity in the aldol condensation of cyclopentanone and *** mono-condensation and bicondensation products were obtained with yield of 95.2%at 100℃.It is found that the synergy effects between amino group of ethanolamine and hydroxyl group of lactic acid play a key role in the aldol *** condensation products were converted into cycloalkanes by HDO over 5%Pd/Nb_(2)O_(5)*** density of the obtained HDO products is 0.89 g/cm^(3)and the freezing point is lower than-60℃.These results suggest that the resulted cycloalkanes can be used as additives to improve the density and low-temperature fluidity of the jet fuels.

关键词： Aldol condensation Cyclopentanone-vanillin Ionic liquid catalysts Hydrodeoxygenation Jet fuel

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Conceptual design and safety characteristics of a new multi-mission high flux research reactor

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Nuclear Science and Techniques 2023年第3期34卷 9-24页

作者： Wei Xu Jian Li Heng Xie Zhi-Hong Liu Jing Zhao Fei Xie Lei Shi School of Nuclear Science and Engineering Beijing Key Laboratory of Passive Safety Technology for Nuclear EnergyNorth China Electric Power UniversityBeijing 102206China Institute of Nuclear and New Energy Technology Collaborative Innovation Center of Advanced Nuclear Energy TechnologyKey Laboratory of Advanced Reactor Engineering and Safety of Ministry of EducationTsinghua UniversityBeijing 100084China

Research reactors with neutron fluxes higher than 10^(14) n cm^(−2) s^(−1) are widely used in nuclear fuel and material irradiation,neutron-based scientific research,and medical and industrial isotope *** high flux research reactors are not only important scientific research facilities for the development of nuclear energy but also represent the national comprehensive technical *** has several high flux research reactors that do not satisfy the requirements of nuclear energy development.A high flux research reactor has the following features:a compact core arrangement,high power density,plate-type fuel elements,a short refueling cycle,and high coolant velocity in the *** characteristics make it difficult to simultaneously realize high neutron flux and optimal safety margin.A new multi-mission high flux research reactor was designed by the Institute of Nuclear and New Energy Technology at Tsinghua University in China;the reactor can simul-taneously realize an average neutron flux higher than 2.0×10^(15) n cm^(−2) s^(−1) and fulfill the current safety *** high flux research reactor features advanced design concepts and has sufficient safety margins according to the preliminary safety *** on the analysis of the station blackout accident,loss of coolant accident,and reactivity accident of a single-control drum rotating out accidently,the maximum temperature of the cladding surface,minimum departure from nucleate boiling ratio,and temperature difference to the onset of nucleate boiling temperature satisfy the design limits.

关键词： High flux research reactor Neutron flux Safety analysis Maximum temperature of cladding surface Departure from nucleate boiling ratio

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Bimetallic catalysts as electrocatalytic cathode materials for the oxygen reduction reaction in microbial fuel cell:A review

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Green Energy & Environment 2023年第4期8卷 1043-1070页

作者： Ke Zhao Yuanxiang Shu Fengxiang Li Guosong Peng College of Municipal and Environmental Engineering Ministry of Education Key Laboratory of Songliao Aquatic EnvironmentJilin Jianzhu UniversityJilin130118China College of Environmental Science and Engineering Ministry of Education Key Laboratory of Pollution Processes and Environmental CriteriaRemediation and Pollution Control for Urban Ecological EnvironmentalNankai UniversityTianjin300350China

Microbial fuel cell(MFC) is one synchronous power generation device for wastewater treatment that takes into account environmental and energy issues, exhibiting promising potential. Sluggish oxygen reduction reaction(ORR) kinetics on the cathode remains by far the most critical bottleneck hindering the practical application of MFC. An ideal cathode catalyst should possess excellent ORR activity, stability, and costeffectiveness, experiments have demonstrated that bimetallic catalysts are one of the most promising ORR catalysts currently. Based on this, this review mainly analyzes the reaction mechanism(ORR mechanisms, synergistic effects), advantages(combined with characterization technologies), and typical synthesis methods of bimetallic catalysts, focusing on the application effects of early Pt-M(M = Fe, Co, and Ni) alloys to bifunctional catalysts in MFC, pointing out that the main existing challenges remain economic analysis, long-term durability and large-scale application, and looking forward to this. At last, the research trend of bimetallic catalysts suitable for MFC is evaluated, and it is considered that the development and research of metal-organic framework(MOF)-based bimetallic catalysts are still worth focusing on in the future, intending to provide a reference for MFC to achieve energy-efficient wastewater treatment.

关键词： Bimetallic catalysts Oxygen reduction reaction Microbial fuel cell Wastewater treatment Power generation

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