Low-Temperature Methanol Synthesis by a Cu-Loaded LaH2+X Electride
Low-Temperature Methanol Synthesis by a Cu-Loaded LaH2+X Electride
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DOI：
10.1021/acscatal.2c03662
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发表时间：
2022-10-02
期刊：
影响因子：
12.9
通讯作者：
Hosono, Hideo
中科院分区：
文献类型：
--
作者：
Sugiyama, Hironobu;Nakao, Takuya;Hosono, Hideo
甲醇是碳一化学中的关键化学品和能源载体。甲醇的工业合成使用非均相催化剂Cu/ZnO/Al 2 O3，在高温和高压的苛刻条件下进行。在这里，我们提出了一种催化剂的设计理念，以实现低温合成甲醇和报告，铜负载稀土金属氧化物（Cu/REH 2 +x）的工作作为有效的催化剂，从CO和H2合成甲醇在温度低于100 ℃，其中传统的Cu/ZnO/Al 2 O3工业催化剂不能很好地工作。这种催化活性是由于源自高度供电子载体材料的带负电荷的Cu位点和与CO直接反应的氢化物离子。催化剂的活化能和转化频率分别比常规Cu基催化剂的活化能和转化频率高不到一半和接近20倍。目前的工作表明，具有低功函数的阴离子电子，支持材料的金属性质，以及支持中的氢化物离子在低温甲醇合成中起着关键作用。
Methanol is a key chemical in C1 chemistry and energy carrier. The industrial synthesis of methanol uses a heterogeneous catalyst, Cu/ZnO/Al2O3, under harsh conditions of high temperature and high pressure. Here, we propose a design concept for a catalyst to achieve low-temperature synthesis of methanol and report that Cu-loaded rare-earth hydrides (Cu/REH2+x) work as effective catalysts for methanol synthesis from CO and H2 at temperatures below 100 degrees C, where the conventional Cu/ZnO/Al2O3 industrial catalyst does not work well. This catalytic activity is due to negatively charged Cu sites that originate from the highly electron -donating support material and hydride ions directly reactive with CO. The activation energy and turn over frequency for the catalyst are less than half and similar to 20 times higher than that for conventional Cu-based catalysts, respectively. The present work demonstrates that anionic electrons with a low work function, the metallic nature of the support material, and hydride ions in the support play key roles for low-temperature methanol synthesis.