Tailored alcohol distribution by non-dissociated CO adsorption strength on engineered Cu sites in syngas conversion

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-11-27 DOI:10.1016/j.jcat.2024.115873

Qi Ping, Yanru Zhu, Jian Zhang, Zhe An, Xin Shu, Hongyan Song, Jing He

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Abstract

The competition and diversity of coinstantaneous elementary reactions in syngas conversion make the production of targeted products with high selectivity much more challenging. This work demonstrates the control of product distribution in syngas conversion by changing the adsorption strength of non-dissociated CO on engineered Cu sites. The strength of non-dissociated CO adsorption has been tailored by atomic-Cu₁ or ensemble-Cu_n on Co₁Ga₁ intermetallic compounds. In syngas conversion, the introduction of either Cu sites could promote the selectivity of alcohols, while atomic-Cu₁ sites enhance the production of methanol and ensemble-Cu_n sites favor the production of C₂₊ alcohol. A strong adsorption of non-dissociated CO occurs on electron-deficient atomic-Cu₁ sites, leading to an increase of alcohols with > 90 % of methanol in alcohols due to direct hydrogenation. A weaker adsorption of non-dissociated CO occurs on ensemble-Cu_n sites, which allows the carbonyl insertion to alkyl species, affording alcohols with ∼ 92 % of C₂₊ alcohol.

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在合成气转化过程中，通过工程设计的 Cu 位点上的非解离 CO 吸附强度调整酒精分布

合成气转化过程中同时发生的基本反应的竞争性和多样性使得生产具有高选择性的目标产品变得更具挑战性。这项工作展示了通过改变非离解一氧化碳在工程铜位点上的吸附强度来控制合成气转化过程中的产物分布。在 Co1Ga1 金属间化合物上，通过原子-Cu1 或集合-Cun 来定制非离解 CO 的吸附强度。在合成气转化过程中，任一 Cu 位点的引入都能提高醇的选择性，而原子-Cu1 位点能提高甲醇的生产，集合-Cun 位点则有利于 C2+ 醇的生产。缺电子的原子-Cu1 位点对非解离 CO 有较强的吸附作用，导致醇类的增加，由于直接加氢，醇类中甲醇的比例达到 90%。在集合-Cun 位点上，非解离 CO 的吸附力较弱，这使得羰基插入到烷基中，从而产生含 ∼ 92 % C2+ 醇的醇。

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来源期刊

Journal of Catalysis 工程技术-工程：化工

CiteScore

12.30

自引率

5.50%

发文量

447

审稿时长

31 days

期刊介绍： The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.