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Highly Selective Electrochemical Reduction of CO2 to CH4 over Vacancy–Metal–Nitrogen Sites in an Artificial Photosynthetic Cell
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-01-16 , DOI: 10.1021/acssuschemeng.9b07258
Xiaoxu Xuan 1 , Jun Cheng 1 , Xiao Yang 1 , Junhu Zhou 1
Affiliation  

Copper-containing materials have been widely researched as promising catalysts for CO2 electrochemical reduction reaction (CO2RR). However, several challenges remain with these materials, such as the aggregation of copper atoms into large-size nanoparticles, which decreases the number of active sites and the catalytic efficiency. Herein, bimetal pyrolyzed zeolite imidazole frameworks (ZIFs) of copper and zinc with various ratios were prepared, in which the aggregation of copper atoms was alleviated. CuN3(I) coordination active sites were fabricated and confirmed by synchrotron radiation spectra. The Cu1Zn1–N–C catalyst with maximum content of CuN3(I) demonstrated high CO2RR product selectivity of 95.6% toward CH4 gas fuel product in an artificial photosynthetic cell. Density functional theory calculations showed that the relative free energy of *CHO was the lowest on CuN3(I) coordination structure for reducing CO2 to CH4, which accounts for the high selectivity of Cu1Zn1–N–C catalyst in CO2RR.

中文翻译:

在人工光合作用细胞中空位,金属,氮位点上高选择性电化学还原CO 2至CH 4

含铜材料已被广泛研究用作CO 2电化学还原反应(CO2RR)的有前途的催化剂。但是,这些材料仍然面临一些挑战,例如将铜原子聚集成大尺寸的纳米颗粒,这会减少活性位点的数量和催化效率。在此,制备了具有不同比例的铜和锌的双金属热解沸石咪唑骨架(ZIF),从而减轻了铜原子的聚集。制备了CuN 3(I)配位活性位点,并通过同步辐射光谱确认。具有最大CuN 3含量的Cu 1 Zn 1 –N–C催化剂(I)在人造光合作用电池中显示出对CH 4气体燃料产品的95.6%的高CO2RR产物选择性。密度泛函理论计算表明,在将CO 2还原为CH 4的CuN 3(I)配位结构上,* CHO的相对自由能最低,这说明Cu 1 Zn 1 –N–C催化剂在CO2RR中具有高选择性。
更新日期:2020-01-17
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