Cu-supported nano-ZrZnOx as a highly active inverse catalyst for low temperature methanol synthesis from CO2 hydrogenation

IF 20.2 1区 化学 Q1 CHEMISTRY, PHYSICAL
Yangzhi Xu , Zirui Gao , Yao Xu , Xuetao Qin , Xin Tang , Zhiwei Xie , Jinrong Zhang , Chuqiao Song , Siyu Yao , Wu Zhou , Ding Ma , Lili Lin
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Abstract

Hydrogenation of CO2 into methanol at low-temperature on Cu-based catalysts is of great significance, but remains challenging to enhance activity. In this paper, we report an inverse catalyst constructed with nano-ZrZnOx supported on Cu particles with outstanding methanol synthesis performance at 220 ℃, two times higher than that of commercial Cu/ZnO/Al2O3 catalysts under the same conditions. Detailed structure characterization and performance evaluation demonstrate that the ZrZnOx mixed oxide serves as the most active oxide-metal interface site for CO2 hydrogenation. The ZrZnOx/Cu inverse catalyst increases the weak and medium CO2 adsorption sites which are further demonstrated responsible to the methanol productivity. In situ DRIFTs studies reveal that the inverse interface accelerates the reduction of asymmetric formate intermediates and prevents the generation of CO. The combination of enhanced CO2 activation capability and accelerated hydrogenation rate of intermediates over the ZrZnOx/Cu inverse catalyst probably contribute to the remarkable methanol synthesis performance from CO2.

Abstract Image

铜支撑纳米氧化锆(Nano-ZrZnOx)作为二氧化碳加氢低温合成甲醇的高活性反相催化剂
在铜基催化剂上低温加氢将 CO2 转化为甲醇具有重要意义,但如何提高其活性仍是一项挑战。本文报告了一种以纳米 ZrZnOx 为载体的反相催化剂,该催化剂在 220 ℃ 下具有优异的甲醇合成性能,是相同条件下商用 Cu/ZnO/Al2O3 催化剂性能的两倍。详细的结构表征和性能评估表明,ZrZnOx 混合氧化物是二氧化碳加氢过程中最活跃的氧化物-金属界面位点。ZrZnOx/Cu 反相催化剂增加了弱和中等 CO2 吸附位点,这进一步证明了其对甲醇生产率的影响。原位 DRIFTs 研究表明,反向界面加速了不对称甲酸酯中间产物的还原,并阻止了 CO 的生成。在 ZrZnOx/Cu 反相催化剂上,二氧化碳活化能力的增强和中间产物氢化速率的加快可能是二氧化碳合成甲醇性能显著提高的原因。
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来源期刊
Applied Catalysis B: Environmental
Applied Catalysis B: Environmental 环境科学-工程:化工
CiteScore
38.60
自引率
6.30%
发文量
1117
审稿时长
24 days
期刊介绍: Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.
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