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Bio-Based Waterborne Poly(Vanillin-Butyl Acrylate)/MXene Coatings for Leather with Desired Warmth Retention and Antibacterial Properties

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Engineering 2024年第5期36卷 250-263页

作者： Jianzhong Ma Li Ma Lei Zhang Wenbo Zhang Qianqian Fan buxing han College of Bioresources Chemical and Materials Engineering Shaanxi University of Science and TechnologyXi’an 710021China Xi’an Key Laboratory of Green Chemicals and Functional Materials Xi’an 710021China College of Chemistry and Chemical Engineering Shaanxi University of Science and TechnologyXi’an 710021China Shaanxi Collaborative Innovation Center of Industrial Auxiliary Chemistry and Technology Shaanxi University of Science and TechnologyXi’an 710021China Institute of Chemistry Chinese Academy of SciencesBeijing 100190China

This study presents a solvent-free,facile synthesis of a bio-based green antibacterial agent and aromatic monomer methacrylated vanillin(MV)using *** resulting MV not only imparted antibacterial properties to coatings layered on leather,but could also be employed as a green alternative to petroleum-based carcinogen styrene(St).Herein,MV was copolymerized with butyl acrylate(BA)to obtain waterborne bio-based P(MV-BA)miniemulsion via miniemulsion ***,MXene nanosheets with excellent photothermal conversion performance and antibacterial properties,were introduced into the P(MV-BA)miniemulsion by ultrasonic *** the gradual solidification of P(MV-BA)/MXene nanocomposite miniemulsion on the leather surface,MXene gradually migrated to the surface of leather coatings due to the cavitation effect of ultrasonication and amphiphilicity of MXene,which prompted its full exposure to light and bacteria,exerting the maximum photothermal conversion efficiency and significant antibacterial *** particular,when the dosage of MXene nanosheets was 1.4 wt%,the surface temperature of P(MV-BA)/MXene nanocomposite miniemulsioncoated leather(PML)increased by about 15℃ in an outdoor environment during winter,and the antibacterial rate against Escherichia coli and Staphylococcus aureus was nearly 100%under the simulated sunlight treatment for 30 ***,the introduction of MXene nanosheets increased the air permeability,water vapor permeability,and thermal stability of these *** study provides a new insight into the preparation of novel,green,and waterborne bio-based nanocomposite coatings for leather,with desired warmth retention and antibacterial *** can not only realize zerocarbon heating based on sunlight in winter,reducing the use of fossil fuels and greenhouse gas emissions,but also improve ability to fight off invasion by harmful bacteria,viruses,and other microorganisms.

关键词： MXene nanosheets Vanillin Styrene substitute Leather coating Photothermal conversion Warmth retention Antibacterial properties

Efficient nitrate electroreduction over Mn-doped Cu catalyst via regulating N-containing intermediates adsorption configuration

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Science China Chemistry 2024年第6期67卷 1969-1975页

作者： Limin Wu Shunhan Jia Libing Zhang Ruhan Wang Jiaqi Feng Xiaofu Sun buxing han Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing100049China College of Chemical Engineering and Environment China University of PetroleumBeijing102249China Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai200062China

The electrochemical reduction of NO_(3)^(-)to NH_(3)holds promise for economic and environmental benefits,presenting an energyefficient alternative to the traditional Haber-Bosch ***,challenges exist due to its sluggish kinetics,multiple intermediates,and various reaction *** this study,Mn-doped-Cu catalyst was synthesized and employed for electrochemical NO_(3)^(-)-to-NH_(3)*** doping of Mn into Cu resulted in exceptional performance,achieving a FE of 95.8%and an NH_(3)yield rate of 0.91 mol g^(-1)h^(-1)at-0.6 V in a neutral electrolyte at low NO_(3)^(-)*** experimental studies and theoretical calculations revealed that the Mn dopant enhanced the kinetic rate of NO_(2)~--to-NH_(3)and induced a distinct configuration of**** alteration decreased the energy barrier of*NO-to-*NOH,consequently promoting the conversion of NO_(3)^(-)-to-NH_(3).

关键词： nitrate reduction electrocatalysis ammonia synthesis N-intermediate green chemistry

CO2/NOx-involved Electrochemical C-N Coupling Reactions

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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES 2024年第5期40卷 764-775页

作者： Sui, Xiqing Wu, Limin Jia, Shunhan Jin, Xiangyuan Sun, Xiaofu han, buxing Chinese Acad Sci Beijing Natl Lab Mol Sci Key Lab Colloid & Interface & Thermodynam Ctr Carbon Neutral ChemInst Chem Beijing 100190 Peoples R China Univ Chinese Acad Sci Sch Chem Sci Beijing 100049 Peoples R China East China Normal Univ Sch Chem & Mol Engn Shanghai Key Lab Green Chem & Chem Proc Shanghai 200062 Peoples R China

With the excessive use of fossil fuels leading to significant CO2 emissions, and the continuous increase of NOx in water bodies and soils, the use of electrochemical methods for the conversion of CO2 and NOx has garnered widespread attention as a green chemical approach due to its advantages of being environmentally friendly, low-carbon, and straightforward. C-N bonds are widely present in many value-added chemicals, such as urea, amides, and oximes. However, traditional methods for constructing C-N bonds typically involve thermochemical processes. Therefore, using electrochemical methods to catalyze the reduction of CO2 and NOx for C-N bond formation has emerged as a green and sustainable alternative. This paper summarizes the research progress of electrochemical C-N bond construction involving CO2 and NOx from the perspectives of reaction mechanisms and catalytic system construction, reviews the electrochemical synthesis of urea, amines, amides, and oximes through electrochemical C-N bond construction, and finally analyzes the current problems and challenges in the field, providing prospects for its future development.

关键词： CO2 reduction NOx reduction C-N coupling Electrocatalysis GAS-DIFFUSION ELECTRODES EFFICIENT UREA ELECTROSYNTHESIS ELECTROCATALYTIC CO2 REDUCTION CARBON-DIOXIDE NITRITE IONS NITRATE REDUCTION AMMONIA-SYNTHESIS BIPOLAR MEMBRANE ELECTROREDUCTION CATALYSTS

Robust Carbon-Carbon Cleavage in Lignin to Produce Phenol and Cyclohexanone

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Chemical Research in Chinese Universities 2024年第1期40卷 29-35页

作者： WANG Lulin CHENG Xiaomeng DONG Minghua LUAN Sen WU Yuxuan han buxing LIU Huizhen Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100190P.R.China University of Chinese Academy of Sciences Beijing 100049P.R.China

The challenge of breaking 5-5'bonds in lignin,attributed to their high bonding energy,has prompted the development of a new transformation ***,an important model compound for lignin,contains these 5-5'bonds,making it crucial to devise a strategy for their cleavage in lignin *** study introduces a novel method for transforming biphenyl,involving selective hydrogenation to cyclohexylbenzene by Ni/SiO2 catalyst,followed by its oxidation to phenol and cyclohexanone through a radical *** demonstrate that the catalysts with small particles have strong catalytic activity,while there is little difference in *** reason for the high selectivity of cyclohexylbenzene is due to the limited adsorption of cyclohexylbenzene on Ni/*** work presents a fresh approach to breaking resilient C-C bonds in lignin.

关键词： Lignin 5-5'Bond Ni/SiO_(2) Phenol

Electrochemical CO_(2)reduction to C_(2+)products over Cu/Zn intermetallic catalysts synthesized by electrodeposition

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Frontiers in Energy 2024年第1期18卷 80-88页

作者： Ting DENG Shuaiqiang JIA Shitao han Jianxin ZHAI Jiapeng JIAO Xiao CHEN Cheng XUE Xueqing XING Wei XIA Haihong WU Mingyuan HE buxing han School of Chemistry and Molecular Engineering East China Normal UniversityShanghai 200062China Institute of Eco-Chongming Shanghai 202162China Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China Institute of Chemistry Chinese Academy of SciencesBeijing 100190China

Electrocatalytic CO_(2)reduction(ECR)offers an attractive approach to realizing carbon neutrality and producing valuable chemicals and fuels using CO_(2)as the ***,the lack of cost-effective electrocatalysts with better performances has seriously hindered its ***,a one-step co-electrodeposition method was used to introduce Zn,a metal with weak^(*)CO binding energy,into Cu to form Cu/Zn intermetallic catalysts(Cu/Zn IMCs).It was shown that,using an H-cell,the high Faradaic efficiency of C_(2+)hydrocarbons/alcohols()could be achieved in ECR by adjusting the surface metal components and the applied *** suitable conditions,FEC_(2+)and current density could be as high as 75%and 40 mA/cm^(2),*** with the Cu catalyst,the Cu/Zn IMCs have a lower interfacial charge transfer resistance and a larger electrochemically active surface area(ECSA),which accelerate the ***,the^(*)CO formed on Zn sites can move to Cu sites due to its weak binding with*CO,and thus enhance the C–C coupling on the Cu surface to form C_(2+)products.

关键词： carbon dioxide electroreduction electrochemistry co-electrodeposition intermetallic catalysts value-added chemicals

Asymmetric Cu Sites for Enhanced CO_(2)Electroreduction to C_(2+)Products

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CCS Chemistry 2024年第5期6卷 1231-1239页

作者： Weiwei Guo Xingxing Tan Shunhan Jia Shoujie Liu Xinning Song Xiaodong Ma Limin Wu Lirong Zheng Xiaofu Sun buxing han Beijing National Laboratory for Molecular Sciences Key Laboratory of Colloid and Interface and ThermodynamicsCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100190 Institute of Molecular Metrology College of Chemistry and Chemical EngineeringQingdao UniversityQingdao 266071 School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049 School of Materials Science and Engineering Anhui UniversityHefei 230601 Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049 Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062

Cu-based electrocatalysts can have excellent activity for the generation of C_(2+)products from a CO_(2)reduction reaction(CO_(2)RR).Cuδ+species is crucial in tuning the performance of the ***,we discovered that Si-doped Cu catalysts had excellent performance for electrochemical CO_(2)to C_(2+)products.A high Faradaic efficiency(FE)of 84.7%was achieved with a current density of 289mA cm^(−2)in the flow-cell *** situ experimental results showed that the significant reconstruction occurred during the electrolysis,resulting in the formation of the asymmetric Cu sites(Cu^(0)-Cu^(+)).The ratio of Cu^(0)and Cu^(+)could be tuned by changing Si *** experiments and theoretical calculations demonstrated that the asymmetric Cu sites caused by the appropriate Si doping promoted CO_(2)activation and strengthened the adsorption of^(*)CO *** was beneficial to the subsequent^(*)CO–^(*)CO dimerization step,and thus,accounted for the enhancement of C_(2+)selectivity.

关键词： carbon dioxide electrocatalysis asymmetric Cu sites C-C coupling green chemistry

Atomically Dispersed Pt and NiO Clusters Synergistically Enhanced C–O Bond Hydrogenolysis

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CCS Chemistry 2024年第3期6卷 709-718页

作者： Junjuan Yang Sen Luan Minghua Dong Yuxuan Wu Xueqing Xing Xingwu Liu Junfeng Xiang Zhijuan Zhao Shaopeng Li Bin Zhang Huizhen Liu buxing han Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijing 100190 School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049 Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsBeijing 100049 National Energy Center for Coal to Liquids Synfuels China Co.Ltd.Huairou DistrictBeijing 101400 Center for Physicochemical Analysis and Measurement Institute of ChemistryChinese Academy of SciencesBeijing 100190 Physical Science Laboratory Huairou National Comprehensive Science CenterUniversity of Chinese Academy of SciencesBeijing 100049

C–Obond activation is a highly efficient,fundamental strategy in the depolymerization and hydrodeoxygenation of chemicals with oxygen-containing functional groups such as oil,coal,and *** efficient catalysts for C–Oactivation with ultralow-loading noble and non-noble metals is highly desirable for the improvement of metal atomic ***,bimetallic catalysts with atomically dispersed Pt and NiO clusters on different supports were fabricated,and the prepared Pt^(δ+)-NiO/Nb_(2)O_(5)and Pt^(δ+)-NiO/TiO_(2)showed outstanding activity for the hydrogenolysis of benzyl phenyl ether with>99%yield of phenol and toluene due to the excellent cooperation of atomically dispersed Pt and NiO *** synergy mechanism between Pt and Ni and their respective roles in the bimetallic catalyst for C–O hydrogenolysis were clearly *** findings deepen our understanding of the synergy of the two active components and are expected to provide new design concepts for the development of multicomponents catalysts.

关键词： bimetallic catalysis synergistic effect C-O bond activation hydrogenolysis hydrogen spillover

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“双碳”背景下的能源电催化技术

科学通报 2024年第25期69卷 3693-3694页

作者：李彦光韩布兴苏州大学功能纳米与软物质研究院苏州215123 中国科学院化学研究所北京100190

在当前能源需求激增和气候变化的背景下,发展契合于“双碳”目标的可再生能源转换技术势在必行.电催化是利用电化学反应促进化学反应过程,在可再生能源的利用和存储方面展现出巨大的潜力.目前,电催化技术在氢气生产/利用、二氧化碳还原... 详细信息

在当前能源需求激增和气候变化的背景下,发展契合于“双碳”目标的可再生能源转换技术势在必行.电催化是利用电化学反应促进化学反应过程,在可再生能源的利用和存储方面展现出巨大的潜力.目前,电催化技术在氢气生产/利用、二氧化碳还原、氮气固定等领域的应用逐渐成为研究的热点,而实现这些电催化技术大规模应用的关键在于先进电催化材料的开发和系统集成.近年来,科技工作者致力于新型电催化材料的设计、反应体系的构建、反应机制的探索等方面的研究,并应用于燃料电池、电解水、含碳/氮燃料循环再生利用等技术中,取得了一些重要的研究成果,有望助力国家“双碳”目标实现.

关键词：电催化二氧化碳还原化学反应过程科技工作者电化学反应可再生能源燃料电池反应机制

Tuning the Surface Field by Embedding Cations into Metals to Direct the Reaction Pathway of CO_(2) Electroreduction

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CCS Chemistry 2024年第3期6卷 631-640页

作者： Pei Zhang Meng Zhou Shiqiang Liu Xueqing Xing Jiahao Yang Peng Chen Yaoyu Yin Yingying Cheng Xing Tong Jun Ma Qinggong Zhu Xiaofu Sun ZhongJun Chen Xinchen Kang buxing han Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100190 Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049 Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062 School of Chemistry University of Chinese Academy of SciencesBeijing 100049

The creation of universal strategies to affect the reaction route of the electroreduction of CO_(2) is ***,we report the first work to introduce cations into diverse metals such as Cu,Bi,In,and Sn via the electroreduction of related metallic oxides in quaternary ammonium surfactant *** to their physical adsorption,cations embedded into the electrodes have a more pronounced impact on the electrical field,which effectively influences the adsorption state of *** the increase of surface field,the hydrogen evolution reaction and*COOH route are significantly reduced,favouring the*OCHO pathway *** a result,hydrogen,CO,and C_(2+)products almost completely vanish at−0.5 V versus RHE in 0.1 M Na_(2)SO_(4)in an H-type cell after enough cations are embedded into the Cu electrode,and the faradaic efficiency of formate rises from 18.0%to 99.5%simultaneously.

关键词： CO_(2)electroreduction tuneable products electrical field reaction pathway cations embedding