Electronic Modulation of a Copper/Zinc Oxide Catalyst by a Heterojunction for Selective Hydrogenation of Carbon Dioxide to Methanol
Electronic Modulation of a Copper/Zinc Oxide Catalyst by a Heterojunction for Selective Hydrogenation of Carbon Dioxide to Methanol
复制标题
通过异质结对铜/氧化锌催化剂进行电子调节，用于二氧化碳选择性加氢制甲醇
DOI：
10.1002/anie.201200903
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发表时间：
2012-01-01
影响因子：
16.6
通讯作者：
Tsang, Shik Chi Edman
中科院分区：
文献类型：
--
作者：
Liao, Fenglin;Zeng, Ziyan;Tsang, Shik Chi Edman
在过去的几十年里，由大气中二氧化碳（CO2）浓度的增加和化石燃料的耗尽引起的全球变暖引起了科学家和政府机构的广泛关注。[1，2]将CO2催化转化为液体燃料或其他有价值的化学品对这些重要的环境和能源问题具有积极影响。[3，4]特别地，CO2加氢为甲醇是非常有吸引力的，因为其作为高能量密度液体燃料和关键的铂基化学品（用于制造甲醛、甲基叔丁基醚和乙酸）的位置。从可再生能源（太阳能、水电、生物质或过量化学热）方便地大规模生产氢气也支持这种新的绿色工艺。[5，6]关于CO2氢化的催化研究的大多数研究已经使用改性的工业甲醇催化剂用于合成气（CO/H2）的氢化，其含有Cu和ZnO作为主要组分以及氧化铝载体和不同的改性剂。[7-9]Ni最近被认为显示出比Cu更高的周转频率。[10]到目前为止，由于缺乏对加氢反应的了解以及对催化剂配方中重要材料相互作用的基本理解，催化剂的开发缓慢。关于合成气的加氢，已经提出了许多模型来定义铜和锌氧化物的活性中心和协同相互作用。[11]例如，ZnO被认为提供溢出氢的活性位点[12]或作为控制铜的分散、形态和比活性的结构导向载体
In the past decades, global warming caused by an increasing concentration of atmospheric carbon dioxide (CO2) and the depletion of fossil fuels have received much attention by scientists and governmental agencies.[1, 2] Catalytic conversion of CO2 to liquid fuels or other valuable chemicals has a positive impact on these important environmental and energy issues.[3, 4] In particular, the hydrogenation of CO2 to methanol is very attractive because of its position as a high energy density liquid fuel and a key platfrom chemical (for manufacture of formaldehyde, methyl-tert-butyl ether, and acetic acid). The convenient production of hydrogen at large scale from renewable energy sources (solar energy, hydropower, biomass, or excess chemical heat) also supports this new green process.[5, 6]The majority of research on catalytic studies of CO2 hydrogenation has been using modified industrial methanol catalysts for the hydrogenation of synthesis gas (CO/H2), which contained Cu and ZnO as the main components together with an alumina support and different modifiers.[7–9] Ni was recently claimed to display a higher turnover frequency than Cu.[10] Up to now, the exploitation of the catalyst is slow because of the lack of knowledge on both hydrogenation reactions and the fundamental understanding of the important material interactions in the catalyst formulation. Regarding the hydrogenation of synthesis gas many models have been proposed to define the active sites and the synergetic interactions of the copper and zinc oxide.[11] For example, ZnO is regarded to provide active sites for spillover hydrogen [12] or as a structure-directing support controlling the dispersion, morphology, and specific activity of the copper