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Siliceous mesocellular foam supported cu catalysts for promoting non-thermal plasma activated CO_(2) hydrogenation toward methanol synthesis

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Frontiers of Chemical Science and Engineering 2024年第7期18卷 55-65页

作者： Yi Chen Shaowei Chen Yan Shao cui Quan Ningbo Gao Xiaolei Fan Huanhao Chen State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China School of Environmental Science and Engineering Nanjing Tech UniversityNanjing 211816China School of Energy and Power Engineering Xi’an Jiaotong UniversityXi’an 710049China Department of Chemical Engineering School of EngineeringThe University of ManchesterManchester M139PLUK Nottingham Ningbo China Beacons of Excellence Research and Innovation Institute University of Nottingham Ningbo ChinaNingbo 315048China Institute of Wenzhou Zhejiang UniversityWenzhou 325006China

Electrified non-thermal plasma (NTP) catalytic hydrogenation is the promising alternative to the thermal counterparts, being able to be operated under mild conditions and compatible with green electricity/hydrogen. Rational design of the catalysts for such NTP-catalytic systems is one of the keys to improve the process efficiency. Here, we present the development of siliceous mesocellular foam (MCF) supported cu catalysts for NTP-catalytic CO_(2) hydrogenation to methanol. The findings show that the pristine MCF support with high specific surface area and large mesopore of 784 m2·g−1 and ~8.5 nm could promote the plasma discharging and the diffusion of species through its framework, outperforming other control porous materials (viz., silicalite-1, SiO_(2), and SBA-15). Compared to the NTP system employing the bare MCF, the inclusion of cu and Zn in MCF (i.e., cu1Zn1/MCF) promoted the methanol formation of the NTP-catalytic system with a higher space-time yield of methanol at ~275 μmol·g_(cat)^(−1)·h^(−1) and a lower energy consumption of 26.4 kJ^(−1)·mmol_(CH_(3)OH)^(-1) (conversely, ~225 μmol·g_(cat)^(−1)·h^(−1) and ~71 kJ^(−1)·mmol_(CH_(3)OH)^(-1), respectively, for the bare MCF system at 10.1 kV). The findings suggest that inclusion of active metal sites (especially Zn species) could stabilize the CO_(2)/CO-related intermediates to facilitate the surface reaction toward methanol formation.

关键词： non-thermal plasma(NTP)catalysis cu catalyst CO_(2)hydrogenation methanol siliceous mesocellular foam(MCF)

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Gas-phase electrocatalytic conversion of CO_2 to chemicals on sputtered cu and cu–C catalysts electrodes

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Journal of Energy Chemistry 2019年第4期28卷 46-53页

作者： N.Gutiérrez-Guerra J.A.González J.C.Serrano-Ruiz E.López-Fernández J.L.Valverde A.de Lucas-Consuegra Departamento de Ingeniería Química Facultad de Ciencias y Tecnologías Químicas Universidad de Castilla-La Mancha Instituto Regional de Investigación Científica Aplicada (IRICA) and Departamento de Física Aplicada Universidad de Castilla-La Mancha Departamento de Ingeniería Universidad Loyola Andalucía

A novel gas-phase electrocatalytic cell containing a low-temperature proton exchange membrane(PEM)was developed to electrochemically convert CO_2into organic *** different cu-based cathode catalysts(cu and cu–C)were prepared by physical vapor deposition method(sputtering)and subsequently employed for the gas-phase electroreduction of CO_2at different temperatures(70–90°C).The prepared electrodes cu and cu–C were characterized by X-ray diffraction(XRD),X-ray photoemission spectroscopy(XPS)and scanning electron microscopy(SEM).As revealed,cu is partially oxidized on the surface of the samples and the cu and cu–C cathodic catalysts were comprised of a porous,continuous,and homogeneous film with nanocrystalline cu with a grain size of 16 and 8 nm,*** influence of the applied current and temperature on the electro-catalytic activity and selectivity of these materials was *** the two investigated electrodes,the pure cu catalyst film showed the highest CO_2specific electrocatalytic reduction rates and higher selectivity to methanol formation compared to the cu–C electrode,which was attributed to the higher particle size of the former and lower cu O/cu *** obtained results show potential interest for the possible use of electrical renewable energy for the transformation of CO_2into valuable products using low metal loading cu based electrodes(0.5 mg cu cm^(-2))prepared by sputtering.

关键词： CO_2 valorization Electro-reduction cu catalyst PEM Selectivity Methanol production

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Syngas to ethanol on Mocu(211)surface:Effect of promoter Mo on C-O bond breaking and C-C bond formation

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Chinese Journal of Chemical Engineering 2022年第5期35卷 78-89页

作者： Lijuan He cuimei Zhi Lixia Ling Riguang Zhang Baojun Wang State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of TechnologyTaiyuan 030024China Key Laboratory of Coal Science and Technology(Taiyuan University of Technology) Ministry of Education and Shanxi ProvinceTaiyuan 030024China College of Chemistry and Bioengineering Taiyuan University of Science and TechnologyTaiyuan 030024China College of Chemistry and Chemical Engineering Taiyuan University of TechnologyTaiyuan 030024China

The mechanism of syngas to ethanol on Mocu(211)surface has been researched by density functional theory(DFT)calculation,and the effects of Mo as a promoter on C-O bond breaking and C-C bond formation have been *** show that cu-Mo atoms constitute the active sites on Mocu(211)surface after Mo atom being served as a promoter of cu *** with cu(211),Mocu(211)has two ***,CH_(3) is the most advantageous monomer on the Mocu(211)surface,which provides abundant CH_(3) intermediate for syngas to ***,the C-C bond is formed mainly by inserting CHO into the abundant CH_(3),and the generated CH_(3)CHO through multiple steps of hydrogenation to generate C_(2)H_(5)*** key of the promoter Mo on the Mocu(211)surface also has been verified by the analysis of its electronic *** charge density shows that the massive electron transfer from Mo to cu,projected density of states(pDOS)shows that the electron transfer from Mo to cu makes the d-band center of Mocu(211)nearer to the Fermi level,these indicate that the Mocu(211)catalytic capacity *** addition of Mo in the cu-based catalyst not only can effectively solve the problem of C-O bond breaking,but also promote C-C bond *** the influence of Mo content on C-O bond breaking and C-C bond formation,compared with Mocu(211),the DFT results and the d-band center of Mo_(2)cu(211)show that the increase of Mo content could not promote the synergistic effect of cu/Mo on the generation of ethanol more effectively.

关键词： Syngas Ethanol DFT cu catalyst Promoter Mo

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Boosting C–C coupling to multicarbon products via high-pressure CO electroreduction

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Journal of Energy Chemistry 2023年第10期85卷 102-107,I0005页

作者： Wenqiang Yang Huan Liu Yutai Qi Yifan Li Yi cui Liang Yu Xiaoju cui Dehui Deng State Key Laboratory of Catalysis Collaborative Innovation Center of Chemistry for Energy MaterialsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Vacuum Interconnected Nanotech Workstation Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123JiangsuChina

Electrochemical CO reduction reaction(CORR) provides a promising approach for producing valuable multicarbon products(C_(2+)), while the low solubility of CO in aqueous solution and high energy barrier of C–C coupling as well as the competing hydrogen evolution reaction(HER) largely limit the efficiency for C_(2+)production in CORR. Here we report an overturn on the Faradaic efficiency of CORR from being HER-dominant to C_(2+)formation-dominant over a wide potential window, accompanied by a significant activity enhancement over a Moss-like cu catalyst via pressuring CO. With the CO pressure rising from 1 to 40 atm, the C_(2+)Faradaic efficiency and partial current density remarkably increase from 22.8%and 18.9 mA cm^(-2)to 89.7% and 116.7 mA cm^(-2), respectively. Experimental and theoretical investigations reveal that high pressure-induced high CO coverage on metallic cu surface weakens the cu–C bond via reducing electron transfer from cu to adsorbed CO and restrains hydrogen adsorption, which significantly facilitates the C–C coupling while suppressing HER on the predominant cu(111) surface, thereby boosting the CO electroreduction to C_(2+)activity.

关键词： CO electroreduction High pressure electrochemistry cu catalyst C–C coupling Multicarbon products

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CO2 electrolysis at industrial current densities using anion exchange membrane based electrolyzers

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Science China Chemistry 2020年第12期63卷 1711-1715页

作者： Pengfei Wei Hefei Li Long Lin Dunfeng Gao Xiaomin Zhang Huimin Gong Guangyan Qing Rui Cai Guoxiong Wang Xinhe Bao State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China

Significant progress on electrocatalytic CO2 reduction reaction (CO2RR) has been achieved in recent ***,the research and development of electrolyzer device for CO2RR is *** we use anion exchange membrane to develop zerogap electrolyzers for *** electrochemical properties of the electrolyzers with Pd/C and cu cathodes are *** Pd/C cathode shows a current density of 200 mA cm^-2with CO Faradaic efficiency of 98%and energy efficiency of 48.8%,while the cu cathode shows a current density of 350 mA cm^-2with total CO2RR Faradaic efficiency of 81.9%and energy efficiency of 30.5%.This work provides a promising demonstration of CO2 electrolyzer using anion exchange membrane for CO2 electrolysis at industrial current densities.

关键词： CO2 electrolysis electrolyzer industrial current density anion exchange membrane energy efficiency Pd/C catalyst cu catalyst

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