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铟作为助剂对纳米晶Cu/CeO催化剂用于CO加氢制甲醇的稳定性和选择性的影响

Influence of Indium as a Promoter on the Stability and Selectivity of the Nanocrystalline Cu/CeO Catalyst for CO Hydrogenation to Methanol.

作者信息

Sharma Sachin Kumar, Paul Bappi, Pal Rohan Singh, Bhanja Piyali, Banerjee Arghya, Samanta Chanchal, Bal Rajaram

机构信息

Light Stock Processing Division, CSIR-Indian Institute of Petroleum, Dehradun 248005, India.

Academy of Scientific and Innovative Research (AcSIR), Ghaziabad 201002, India.

出版信息

ACS Appl Mater Interfaces. 2021 Jun 23;13(24):28201-28213. doi: 10.1021/acsami.1c05586. Epub 2021 Jun 13.

Abstract

Stable catalyst development for CO hydrogenation to methanol is a challenge in catalysis. In this study, indium (In)-promoted Cu nanoparticles supported on nanocrystalline CeO catalysts were prepared and explored for methanol production from CO. In-promoted Cu catalysts with ∼1 wt % In loading showed a methanol production rate of 0.016 mol g h with 95% methanol selectivity and no loss of activity for 100 h. It is found that the addition of indium remarkably increases Cu dispersion and decreases Cu particle size. In addition led to an increased metal-support interaction, which stabilizes Cu particles against sintering during the reaction, leading to high stability and activity. In addition, density functional theory calculations suggested that the reaction is proceeding via reverse water gas shift (RWGS) mechanism where the presence of In stabilized intermediate species and lowered CO activation energy barriers.

摘要

开发用于将CO加氢制甲醇的稳定催化剂是催化领域的一项挑战。在本研究中,制备了负载在纳米晶CeO催化剂上的铟(In)促进的铜纳米颗粒,并探索了其用于由CO生产甲醇的性能。铟负载量约为1 wt%的In促进的Cu催化剂显示出甲醇产率为0.016 mol g⁻¹ h⁻¹,甲醇选择性为95%,并且在100小时内没有活性损失。研究发现,铟的添加显著增加了Cu的分散度并减小了Cu颗粒尺寸。此外,还导致了金属-载体相互作用增强,这使得Cu颗粒在反应过程中不易烧结,从而具有高稳定性和活性。此外,密度泛函理论计算表明,该反应通过逆水煤气变换(RWGS)机理进行,其中In的存在稳定了中间物种并降低了CO活化能垒。

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