CO2 Hydrogenation to Methanol on Indium Oxide-Supported Rhenium Catalysts: The Effects of Size,ACS Catalysis

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CO2 Hydrogenation to Methanol on Indium Oxide-Supported Rhenium Catalysts: The Effects of Size
ACS Catalysis ( IF 11.3 ) Pub Date : 2022-10-04 , DOI: 10.1021/acscatal.2c03709
Chenyang Shen _{1,

2} , Kaihang Sun ₁ , Rui Zou _{1,

2} , Qinglei Wu _{1,

2} , Donghai Mei ₃ , Chang-jun Liu _{1,

2}

Affiliation

In this work, CO₂ hydrogenation over In₂O₃-supported rhenium (Re) catalysts was found to be highly size-dependent. When the Re loading was less than 1 wt %, the strong interaction between Re and In₂O₃ caused atomically dispersed Re species with a positive charge, resulting in high activity for CO₂ hydrogenation to methanol with enhanced stability at elevated temperatures. The space–time yield of methanol over the 1 wt % Re/In₂O₃ catalyst reached 0.54 g_MeOH g_cat^–1 h^–1 with a methanol selectivity of 72.1% at 5 MPa and 573 K. With increasing Re loading, the In₂O₃ supported Re catalysts become more favored for CO₂ methanation. Under the same experimental conditions, the methane selectivity is close to 100.0% over the 10 wt % Re/In₂O₃ catalyst. Catalyst characterizations and density functional theoretical (DFT) calculations further confirm that the size of the Re/In₂O₃ catalyst has a significant effect on hydrogen activation and the selectivity of the CO₂ hydrogenation reaction. Due to the strong Re–In₂O₃ interaction, the atomically dispersed Re in the In₂O₃ surface lattice not only stabilizes oxygen vacancies but also results in H^δ+ formation upon hydrogen adsorption. This significantly promotes methanol synthesis from CO₂ hydrogenation. Meanwhile, the 10 wt % Re/In₂O₃ catalyst with supported Re nanoclusters induces H^δ- formation, which eventually leads to more methane production. The present study demonstrates the atomically dispersed Re/In₂O₃ catalyst is promising for CO₂ hydrogenation to methanol.

中文翻译：

氧化铟负载铼催化剂上 CO2 加氢制甲醇：尺寸的影响

在这项工作中，发现在 In ₂ O ₃负载的铼 (Re) 催化剂上的CO _{2加氢高度依赖于尺寸。}当 Re 负载量小于 1 wt% 时，Re 和 In ₂ O ₃之间的强相互作用导致具有正电荷的原子分散的 Re 物种，导致 CO ₂加氢制甲醇的高活性，并在高温下增强稳定性。_{在 1 wt % Re/In 2} O ₃催化剂上甲醇的时空产率达到 0.54 g _MeOH g _cat^–1 h ^–1在 5 MPa 和 573 K 条件下甲醇选择性为 72.1%。随着 Re 负载量的增加，In ₂ O ₃负载的 Re 催化剂对 CO ₂甲烷化变得更有利。_{在相同的实验条件下，10 wt% Re/In 2} O ₃催化剂的甲烷选择性接近100.0% 。催化剂表征和密度泛函理论（DFT）计算进一步证实了Re/In ₂ O _{3催化剂的尺寸对氢气活化和CO}₂加氢反应的选择性有显着影响。由于强 Re-In ₂ O ₃相互作用，In ₂ O ₃表面晶格中原子分散的 Re 不仅稳定了氧空位，而且在氢吸附时导致 H ^{δ+的形成。}这显着促进了由CO ₂加氢合成甲醇。同时，负载有 Re 纳米团簇的 10 wt% Re/In ₂ O ₃催化剂诱导 H ^{δ -}的形成，最终导致更多的甲烷产生。本研究表明原子分散的 Re/In ₂ O ₃催化剂有望用于 CO ₂加氢制甲醇。

更新日期：2022-10-04

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