通过热还原调整 PdIn/CeO2 双金属催化剂的活性,以改善通过二氧化碳加氢合成甲醇的工艺

IF 3.5 3区 工程技术 Q2 ENGINEERING, CHEMICAL AIChE Journal Pub Date : 2024-09-25 DOI:10.1002/aic.18617
Yan Shao, Bohong Wu, Boya Qiu, Rongsheng Cai, Cui Quan, Ningbo Gao, Feng Zeng, Xiaolei Fan, Huanhao Chen
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引用次数: 0

摘要

Pd-In2O3 协同催化剂是通过 CO2 加氢制取甲醇的理想候选催化剂,其中的金属相可以通过热还原处理进行调整,从而显著影响催化活性。本研究对热还原温度对支撑在 CeO2 上的 Pd 和 In2O3 相(即 PdIn/CeO2)的变化和相互作用的影响及其与 CO2 加氢合成甲醇的相关性进行了全面研究。研究结果表明,富含 Pd/In 的 PdIn 合金和相互作用相对较强的 In2O3 是促进甲醇形成的关键相(通过在 300°C 下还原 PdIn/CeO2),从而使甲醇的选择性高达 78.9%,时空产率 (STY) 为 3.6 gCH3OH gPdIn-1 h-1。还原温度的进一步提高(从 300°C 提高到 500°C)促进了均质化 PdIn 金属间合金的形成,但其解离 H2 和活化 CO2 的能力明显较差,因此甲醇产率也较低。
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Activity of bimetallic PdIn/CeO2 catalysts tuned by thermal reduction for improving methanol synthesis via CO2 hydrogenation
Synergistic Pd–In2O3 catalysts are promising candidates for producing methanol via CO2 hydrogenation, and the metal phases in them can be tuned by thermal reduction treatment affecting the catalytic activity significantly. This work presents a comprehensive investigation to gain an insight into the effect of thermal reduction temperature on the variation and interaction of Pd and In2O3 phases supported on CeO2 (viz., PdIn/CeO2) and their correlations with CO2 hydrogenation toward methanol synthesis. The findings show that Pd/In-rich PdIn alloys and In2O3 with relatively strong interaction are key phases (by reducing the PdIn/CeO2 at 300°C) for promoting methanol formation, leading to a high selectivity to methanol at 78.9% and space–time yield (STY) of 3.6 gCH3OH gPdIn−1 h−1. A further increase in reduction temperature (from 300 to 500°C) promoted the formation of homogenized PdIn intermetallic alloys with significantly poor ability for H2 dissociation and CO2 activation, and hence poor methanol yield.
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来源期刊
AIChE Journal
AIChE Journal 工程技术-工程:化工
CiteScore
7.10
自引率
10.80%
发文量
411
审稿时长
3.6 months
期刊介绍: The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.
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