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Tandem electrocatalysis for CO2 reduction to multi-carbons

Science China Chemistry 2024年第11期67卷 3631-3651页

作者： Xindi Li Tianxiang Yan Yichen Meng Zhanpeng Liang Tianying Zhang Haoyuan Chi Ziting Fan Yifan Jin Haoran Zhang Sheng Zhang Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Centre of Chemical Science and Engineering School of Chemical Engineering and Technology Tianjin University Joint School of National University of Singapore and Tianjin University International Campus of Tianjin University Haihe Laboratory of sustainable Chemical Transformations

The rising CO2concentration in the atmosphere due to extensive use of fossil fuels has led to serious climate and environmental issues. One efficient solution is that CO2capture from industrial emissions followed its conversion into value-added chemicals driven by renewable energies. CO2electroreduction（CO2RR） features a green and sustainable fashion towards effective CO2conversion, but still suffers from low multi-carbon selectivity and yield. Considering the pivotal role of CO intermediate in C–C coupling to multi-carbon formation, tandem CO2RR systems with separated CO generation and consumption components could facilitate the coupling between *CO-based intermediates to energy-intensive multi-carbons by manipulating CO diffusion and surface coverage. In this aspect, we comprehensively reviewed the design principles of tandem systems for CO2electroreduction reaction. The chemistry behind the C–C coupling regarding to their distribution and diffusion was initially introduced, which was followed by achievements on tandem architectures, from catalysts, electrodes to systems. Future directions and perspectives on advanced tandem system designs for CO2RR were discussed at the end. This review contributes to the understanding of structureperformance correlations in tandem catalysis and helps guide the effective collection of multi-carbons of high-yield and highselectivity.

关键词： electrocatalytic CO2 reduction tandem electrocatalysis design CO mass transfer model

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Patterns and mechanisms of belowground carbon responses to changes in precipitation

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Journal of Plant Ecology 2024年第2期17卷 1-17页

作者： Hongyang Chen Qi Zhang Lingyan Zhou Xuhui Zhou School of Forestry Key Laboratory of Sustainable Forest Ecosystem Management-Ministry ofEducationNortheast Forestry UniversityHarbin 150040China Research Center Shanghai Botanical Garden/Shanghai Engineering Research Center of Sustainable Plant InnovationShanghai 200231China

It is well known that aboveground productivity usually increases with ***,how belowground carbon(C)processes respond to changes in precipitation remains elusive,although belowground net primary productivity(BNPP)represents more than one-half of NPP and soil stores the largest terrestrial C in the *** paper reviews the patterns of belowground C processes(BNPP and soil C)in response to changes in precipitation from transect studies,manipulative experiments,modeling and data integration and *** results suggest the possible existence of nonlinear patterns of BNPP and soil C in response to changes in precipitation,which is largely different from linear response for aboveground productivity.C allocation,root turnover time and species composition may be three key processes underlying mechanisms of the nonlinear responses to changes in precipitation for belowground C *** addition,microbial community structure and long-term ecosystem processes(*** assemblage,soil texture,aggregate stability)may also affect patterns of belowground C processes in response to changes in *** last,we discuss implications and future perspectives for potential nonlinear responses of belowground C processes to changes in precipitation.

关键词： belowground processes BNPP nonlinear precipitation soil C

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Energy flexibility and resilience analysis of demand-side energy efficiency measures within existing residential houses during cold wave event

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Building Simulation 2024年第7期17卷 1043-1063页

作者： Xiaoyi Zhang Fu Xiao Yanxue Li Yi Ran Weijun Gao innovation Institute for sustainable Maritime Architecture Research and Technology Qingdao University of TechnologyQingdaoChina Department of Building Environment and Energy engineering The Hong Kong Polytechnic UniversityHong KongChina Faculty of Environmental engineering The Universityof KitakyushuKitakyushuJapan

Using the behind-meter data,this study applied a comparison and optimization-based framework to evaluate the energy flexibility and resilience of distributed energy resources within existing houses during cold wave *** analysis demonstrates the effectiveness of high envelope insulation level in improving energy resilience,identifies impacts of distributed energy resources on variations of household electricity ***,a 14.6%reduction in the median value of the normalized load of building group with low U-values,implementations of cogeneration system effectively suppressed variations of electricity *** energy performances of on-site generators are evaluated based on high resolution data,energy flexibility of domestic hot water and thermostatically controlled loads were investigated through built demand response *** reveal that electrifying hot water demand offers additional power flexibility,the integration of fuel cell cogeneration system has proven to be an efficient energy resource,enabling on-site generation of both electricity and hot water,substantially reducing grid *** extreme cold event resulted in significant spikes in space heating power *** optimization results demonstrate that reducing the indoor setpoint temperature effectively decreases daily power consumption by approximately 5.0%per degree *** findings help acquire better understanding of interconnections between energy efficiency and resilience of residential energy-efficient measures.

关键词： system modeling energy efficiency energy resilience cold wave thermal comfort

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A solubility limited pyrene-4,5,9,10-tetraone-based covalent organic framework for high-performance aqueous zinc-organic batteries

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Nano Research 2024年第6期17卷 5095-5103页

作者： Min Cheng Shibing Zheng Tianjiang Sun Diantao Li Weijia Zhang Zhengtai Zha Qiong Sun Jing Tian Kai Zhang Zhanliang Tao Frontiers Science Center for New Organic Matter State Key Laboratory of Advanced Chemical Power SourcesKey Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Renewable Energy Conversion and Storage CentreNankai UniversityTianjin 300071China Haihe Laboratory of sustainable Chemical Transformations Tianjin 300192China

Pyrene-4,5,9,10-tetraone(PTO),with a high theoretical capacity of 408 mAh·g^(−1),is a promising candidate for rechargeable aqueous zinc-ion batteries(RAZIBs),but its zincated products during discharge process suffer from high solubility in ***,aβ-ketoenamine-linked two-dimensional(2D)covalent organic framework(COF)based on a 2,7-diaminopyrene-4,5,9,10-tetraone(4KT-BD)monomer and a 2,4,6-trihydroxy-benzene-1,3,5-tricarbaldehyde(Tp)node(4KT-Tp-COF)is synthesized to address the above *** well-designed 4KT-Tp-COF displays low solubility in 3 M Zn(CF3SO3)2 owing to the favorableπ-πstacking as well as extended ***,the ingenious structural design of the active molecule and the long-range ordered nano-channels alter the intramolecular electron distribution,which facilitates the ionic ***,the 4KT-Tp-COF cathode exhibits a stable capacity of 181 mAh·g^(−1)at 0.2 A·g^(−1),superior rate capability of 139 mAh·g^(−1)at 20 A·g^(−1),and a long lifetime of 1000 cycles without capacity loss at 30 A·g^(−1).Even at a low temperature of−20°C,the electrode also performs an ultralong cycling life of 9000 cycles with a capacity of 106 mAh·g^(−1)at 5 A·g^(−1).The comprehensive characterizations of ex-situ analyses together with the theoretical calculations validate that the groups of C=O can contribute highly accessible redox-active sites for Zn^(2+)*** ultra-stable 4KT-Tp-COF cathode provides important insights for designing robust organic electrodes for sustainable and large-scale electrochemical energy storage.

关键词： pyrene-4,5,9,10-tetraone solubility limited covalent organic framework zinc batteries

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Advanced 2D molybdenum disulfide for green hydrogen production: Recent progress and future perspectives

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Frontiers in Energy 2024年第3期18卷 308-329页

作者： Meng FANG Yuqin PENG Puwei WU Huan WANG Lixin XING Ning WANG Chunmei TANG Ling MENG Yuekuan ZHOU Lei DU Siyu YE Huangpu Hydrogen Energy innovation centre School of Chemistry and Chemical EngineeringGuangzhou UniversityGuangzhou 510006China sustainable Energy and Environment Thrust Function HubThe Hong Kong University of Science and Technology(Guangzhou)Guangzhou 511400China Department of Mechanical and Aerospace engineering The Hong Kong University of Science and TechnologyHong KongChina SinoHykey Technology Company Ltd. Guangzhou 510760China

The development of renewable and affordable energy is crucial for building a sustainable society. In this context, establishing a sustainable infrastructure for renewable energy requires the integration of energy storage, specifically use of renewable hydrogen. The hydrogen evolution reaction (HER) of electrochemical water splitting is a promising method for producing green hydrogen. Recently, two-dimensional nanomaterials have shown great promise in promoting the HER in terms of both fundamental research and practical applications due to their high specific surface areas and tunable electronic properties. Among them, molybdenum disulfide (MoS2), a non-noble metal catalyst, has emerged as a promising alternative to replace expensive platinum-based catalysts for the HER because MoS_(2)has a high inherent activity, low cost, and abundant reserves. At present, greatly improved activity and stability are urgently needed for MoS_(2)to enable wide deployment of water electrolysis devices. In this regard, efficient strategies for precisely modifying MoS_(2)are of interest. Herein, the progress made with MoS_(2)as an HER catalyst is reviewed, with a focus on modification strategies, including phase engineering, morphology design, defect engineering, heteroatom doping, and heterostructure construction. It is believed that these strategies will be helpful in designing and developing high-performance and low-cost MoS2-based catalysts by lowering the charge transfer barrier, increasing the active site density, and optimizing the surface hydrophilicity. In addition, the challenges of MoS_(2)electrocatalysts and perspectives for future research and development of these catalysts are discussed.

关键词： molybdenum disulfide(MoS_(2)) hydrogen evolution reaction(HER) active site electrocatalyst modification strategie

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Graphene-anchored sodium single atoms:A highly active and stable catalyst for transesterification reaction

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Nano Research 2024年第6期17卷 4979-4985页

作者： Song-Song Peng Yao Nian Xing-Ru Song Xiang-Bin Shao Chen Gu Zhi-Wei Xing Shi-Chao Qi Peng Tan You Han Xiao-Qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical engineering Jiangsu National Synergetic Innovation Center for Advanced Materials(SICAM)College of Chemical EngineeringNanjing Tech University30 South Puzhu RoadNanjing 211816China School of Chemical engineering and Technology Tianjin UniversityTianjin 300072China Haihe Laboratory of sustainable Chemical Transformations Tianjin 300192China

Solid strong base catalysts have received considerable attention in various organic reactions due to their facile separation,neglectable corrosion,and environmental *** great progress has been made in the preparation of solid strong base catalysts,it is still challenging to avoid basic sites aggregation on support and active sites loss in reaction ***,we report a tandem redox strategy to prepare Na single atoms on graphene,producing a new kind of solid strong base catalyst(Na1/G).The base precursor NaNO_(3)was first reduced to Na2O by graphene(400℃)and successively to single atoms Na anchored on the graphene vacancies(800℃).Owing to the atomically dispersed of basicity,the resultant catalyst presents high activity toward the transesterification of methanol and ethylene carbonate to synthesize dimethyl carbonate(turnover frequency(TOF)value:125.7 h^(−1)),which is much better than the conventional counterpart Na2O/G and various reported solid strong bases(TOF:1.0-90.1 h^(−1)).Furthermore,thanks to the basicity anchored on graphene,the Na1/G catalyst shows excellent durability during *** work may provide a new direction for the development of solid strong base catalysts.

关键词： solid strong base catalyst basic sites redox graphene single Na atoms

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Subnanometric bimetallic Pt-Pd clusters in zeolites for efficient hydrogen production and selective tandem hydrogenation of nitroarenes

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Science China Chemistry 2024年第9期67卷 2911-2917页

作者： Jiafu Li Tao Cai Yanran Feng Xia Liu Ning Wang Qiming Sun Institute of sustainable Energy and Resources College of Chemistry and Chemical EngineeringKey Laboratory of Shandong Provincial Universities for Functional Molecules and MaterialsQingdao UniversityQingdao 266071China innovation Center for Chemical Sciences College of ChemistryChemical Engineering and Materials ScienceJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123China

The solvolysis of ammonia borane(AB)and the hydrogenation of nitroarenes represent significant reactions for hydrogen generation and value-added chemical *** strategic engineering of the catalysts is imperative for surmounting obstacles associated with their stability and catalytic *** this work,subnanometric bimetallic Pt–Pd clusters were encapsulated within silicalite-1(S-1)zeolites through a ligand-protected in-situ hydrothermal synthesis *** synergetic effect of bimetallic composition and zeolite confinement markedly enhances the catalytic performance of representative Pt_(0.5)Pd_(0.5)@S-1-H catalyst,affording exceptional turnover frequency(TOF)values of 1,043 and 573 mol_(H_(2))mol_(metal)^(-1)min^(-1)for AB hydrolysis and methanolysis at ambient conditions,respectively,surpassing most of the state-of-the-art Pt-based *** and isotopic experiments reveal that the bimetallic catalytic system remarkably boosts the O-H cleavage of water,thereby facilitating the H_(2) production from AB ***,a conspicuous synergistic effect is demonstrated in the shape-selective tandem hydrogenation of nitroarenes,with the bimetallic catalyst facilitating both AB hydrolysis and nitroarene hydrogenation,giving a high TOF value of 1,260 h^(-1)under atmospheric *** study not only demonstrates the effectiveness of bimetallic nanocatalysts encapsulated in zeolites for hydrogen production from chemical hydrogen storage materials,but also paves the way for the design of catalysts with multifunctional active sites capable of synergistically promoting tandem catalytic processes.

关键词： subnanometer bimetallic cluster zeolite synergistic effect ammonia borane solvolysis selective tandem hydrogenation

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Multi-objective Design of Blending Fuel by Intelligent Optimization Algorithms

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Transactions of Tianjin University 2024年第3期30卷 221-237页

作者： Ruichen Liu Cong Li Li Wang Xiangwen Zhang Guozhu Li Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Collaborative innovation Center of Chemical Science and engineering(Tianjin) Tianjin 300072China Haihe Laboratory of sustainable Chemical Transformations Tianjin 300192China

Fuel design is a complex multi-objective optimization problem in which facile and robust methods are urgently ***,a complete workflow for designing a fuel blending scheme is presented,which is theoretically supported,efficient,and *** on the data distribution of the composition and properties of the blending fuels,a model of polynomial regression with appropriate hypothesis space was *** parameters of the model were further optimized by different intelligence algorithms to achieve high-precision ***,the design of a blending fuel was described as a multi-objective optimization problem,which was solved using a Nelder–Mead algorithm based on the concept of Pareto ***,the design of a target fuel was fully validated by *** study provides new avenues for designing various blending fuels to meet the needs of next-generation engines.

关键词： Multi-objective optimization Machine learning Blending fuel

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Effect of ambient pressures on laser-induced breakdown spectroscopy signals

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Frontiers of physics 2024年第4期19卷 243-256页

作者： Kaifan Zhang Weiran Song Zongyu Hou Zhe Wang State Key Laboratory of Power System Operation and Control Tsinghua-Rio Tinto Joint Research Centre for ResourcesEnergy and Sustainable DevelopmentInternational Joint Laboratory on Low Carbon Clean Energy InnovationInstitute for Carbon NeutralityDepartment of Energy and Power EngineeringTsinghua UniversityBeijing 100084China Shanxi Research Institute for Clean Energy Tsinghua UniversityTaiyuan 030032China

Laser-induced breakdown spectroscopy(LIBS)is regarded as the future superstar for analytical chemistry and widely applied in various *** the quality of LIBS signal is fundamental to achieving accurate quantification and large-scale commercialization of *** propose control methods that improve LIBS signal quality,it is essential to have a comprehensive understanding of the influence of key parameters,such as ambient gas pressure,temperature,and sample temperature on LIBS *** date,extensive research has been carried ***,different researchers often yield significantly different experimental results for LIBS,preventing the formation of consistent *** greatly prevents the understanding of influencing laws of key parameters and the improvement of LIBS quantitative *** ambient gas pressure as an example,this paper compares the effects of ambient gas pressure under different optimization conditions,reveals the influence of spatiotemporal window caused by inherent characteristics of LIBS signal sources,i.e.,intense temporal changes and spatial non-uniformity of laser-induced plasmas,on the impact patterns of key *** the perspective of plasma spatiotemporal evolution,the paper elucidates the influence patterns of ambient gas pressure on LIBS signals,clarifying seemingly contradictory research results in the literature.

关键词： laser-induced breakdown spectroscopy spatiotemporal window pressure condition signal uncertainty plasma modulation

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Eco-friendly synthesis and environmental impact assessment of hierarchical Beta zeolite from kaolinite and recycled mother liquor

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Green Chemical engineering 2024年第4期5卷 501-510页

作者： Guoxi Xiao Xiaoling Chen Tiesen Li Chan Wang Qingyan Cui Yuanyuan Yue National engineering Research Center of Chemical Fertilizer Catalyst College of Chemical EngineeringFuzhou University Qingyuan innovation Laboratory

The development of sustainable techniques to produce high-performance zeolite is essential to achieve green production in industry. Herein, we report an eco-friendly route to synthesizing hierarchical Beta zeolite from kaolinite and recycled mother liquor. The results reveal that the unutilized species（such as silicon species and Na+） in mother liquor stayed in a stable concentration during eleven recycled experiments. Moreover, the synthesized Beta zeolites still have comparable physicochemical properties and catalytic performance in the esterification of levulinic acid with ethanol over the initial zeolite although eleven recycled experiments. Life cycle assessment exhibits that the synthesis of Beta zeolite with recycled mother liquor can reduce global warming potential by 23% and resource depletion-water use by 36% compared to that without recycled mother liquor. This quantitatively demonstrates that the approach proposed in this work is really a sustainable one, extremely increasing the utilization efficiency of raw materials and decreasing the environmental burden.

关键词： Eco-friendly synthesis Hierarchical Beta zeolite Recycled mother liquor Life cycle assessment

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