Department of Chemistry, Korea Advanced Institute of Science and Technology, and Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (ibs), Daejeon, 34141, Republic of Korea.
Department of Chemistry, Mokpo National University, Jeonnam, 58554, Republic of Korea.
Nat Commun. 2017 Nov 7;8(1):1156. doi: 10.1038/s41467-017-01165-4.
Developing catalytic systems with high efficiency and selectivity is a fundamental issue for photochemical carbon dioxide conversion. In particular, rigorous control of the structure and morphology of photocatalysts is decisive for catalytic performance. Here, we report the synthesis of zinc oxide-copper(I) oxide hybrid nanoparticles as colloidal forms bearing copper(I) oxide nanocubes bound to zinc oxide spherical cores. The zinc oxide-copper(I) oxide nanoparticles behave as photocatalysts for the direct conversion of carbon dioxide to methane in an aqueous medium, under ambient pressure and temperature. The catalysts produce methane with an activity of 1080 μmol g h, a quantum yield of 1.5% and a selectivity for methane of >99%. The catalytic ability of the zinc oxide-copper(I) oxide hybrid catalyst is attributed to excellent band alignment of the zinc-oxide and copper(I) oxide domains, few surface defects which reduce defect-induced charge recombination and enhance electron transfer to the reagents, and a high-surface area colloidal morphology.
开发高效和选择性的催化体系是光化学二氧化碳转化的一个基本问题。特别是,严格控制光催化剂的结构和形态对于催化性能至关重要。在这里,我们报告了氧化锌-氧化亚铜混合纳米粒子的合成,其以胶体形式存在,氧化亚铜纳米立方体形貌结合在氧化锌球形核上。氧化锌-氧化亚铜纳米粒子在环境压力和温度下,在水相介质中将二氧化碳直接转化为甲烷,表现出光催化活性。催化剂产生甲烷的活性为 1080 μmol·g-1·h-1,量子产率为 1.5%,甲烷选择性>99%。氧化锌-氧化亚铜混合催化剂的催化能力归因于氧化锌和氧化亚铜区域的优异能带排列,减少了缺陷诱导的电荷复合并增强了电子转移到试剂的表面缺陷少,以及高表面积胶体形态。