工况条件下富氢气体中CO选择性氧化反应的耐受性调控及作用机制研究

doi:10.6023/A24020056

化学学报 ›› 2024, Vol. 82 ›› Issue (7): 819-832.DOI: 10.6023/A24020056 上一篇

综述

工况条件下富氢气体中CO选择性氧化反应的耐受性调控及作用机制研究

王力鹏, 曹道帆, 刘雪, 李超, 刘科^*()

南方科技大学理学院化学系深圳 518055

投稿日期:2024-02-20 发布日期:2024-05-30

作者简介:

王力鹏, 南方科技大学理学院化学系博士研究生, 化学专业; 硕士毕业于华侨大学化工学院环境科学与工程专业, 研究方向大气污染控制工程. 目前已以第一作者分别在J. Catal., Appl. Surf. Sci., Chem. Comm.期刊发表环境催化类研究论文, 当前课题为富氢气体中CO选择性氧化催化剂研发.

刘科, 博士生导师, 澳大利亚国家工程院外籍院士, 南方科技大学创新创业学院院长, 南方科技大学理学院讲席教授, 中国与全球化智库常务理事, 国家海外高层次人才联谊会副会长, 美国化学工程师协会(AIChE)会士, 国际氢能协会(IHA)理事. 主要研究方向为洁净煤技术、新型催化剂的设计合成及其应用、土壤修复与改良、系统仿真模拟与集成.

基金资助:
深圳市科技计划项目, 深圳市科技创新委员会(KQTD20180411143418361); 深圳燃气-南科大联合能源实验室; 广东省催化化学重点实验室-南方科技大学(2020B121201002); 国家自然科学基金(U22B20149)

Effect of Realistic Operating Considerations on Preferential Oxidation of CO and Regulatory Strategies: A Review and Perspectives

Lipeng Wang, Daofan Cao, Xue Liu, Chao Li, Ke Liu^*()

Department of Chemistry, College of Science, Southern University of Science and Technology, Shenzhen 518055, China

Received:2024-02-20 Published:2024-05-30
Contact: *E-mail: liuk@sustech.edu.cn; Tel.: 0755-88010097
Supported by:
Shenzhen Science and Technology Program, Shenzhen Science and Technology Innovation Committee(KQTD20180411143418361); Shenzhen Gas & SUSTech Joint Energy Lab, Southern University of Science and Technology, Guangdong Provincial Key Laboratory of Catalysis(2020B121201002); National Natural Science Foundation of China(U22B20149)

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摘要/Abstract

一氧化碳选择性氧化(CO-PROX)是纯化富氢气体耦合燃料电池发电的关键步骤, CO-PROX能够通过催化作用优先氧化脱除重整气中的CO杂质, 将CO浓度降低至0.001%或0.010%以下, 为燃料电池系统供给高纯H₂提供了技术选择. 在多数的文献研究工作中, 研究者一般采用模拟的重整气组分来评估新型催化剂材料的活性, 设置出理想的CO-PROX反应气氛(惰性气体作为配气代替重整尾气中的CO₂和H₂O, 模拟较低的H₂比例等), 使研究的科学问题更加集中具体, 然而少有研究综合考虑实际工况因素的影响、反应器设计、传质传热、反应器单元衔接等问题. 本研究综述侧重考察调研了H₂O和CO₂对CO-PROX反应的作用, 以及实际工况下可能存在的其他因素的影响, 概括分析了上述因素对CO-PROX反应的抑制/促进作用, 同时归纳整理了提升耐受性的可行调控策略, 为CO-PROX领域的基础研究和工程应用衔接提供重要参考依据.

关键词: CO选择性氧化, H₂O与CO₂影响, 抑制/促进作用, 调控改性策略

In the realm of hydrogen production for fuel cell applications, H₂ must be refined to ultra-high purity levels essential for the functionality of fuel cells. Various methods are available for removing trace contaminants from effluent gas streams, falling into the broad categories of adsorption, membranes, scrubbers, and selective reactions. Preferential oxidation of carbon monoxide (CO-PROX) plays a pivotal role in ensuring the purity of hydrogen-rich gases. This catalytic process selectively removes CO impurities, typically requiring reduction to concentrations below 0.001%, thereby enabling the supply of high-purity H₂ to fuel cells. While much existing research utilizes idealized conditions and simulated reformate gas compositions for evaluating novel CO-PROX catalyst materials, it tends to somewhat overlook the real operational factors (water vapor and carbon dioxide), reactor design, and mass/heat transfer. Unlike the singular improvement of catalytic performance under ideal experimental conditions, the practical application of CO-PROX necessitates consideration of unavoidable factors, such as the upstream hydrogen source and the downstream anode tolerance of fuel cell. It is also imperative to design an optimized CO-PROX reactor that takes into account realistic operating conditions. This comprehensive review delves into the multifaceted aspects of CO-PROX, mainly focusing on the impact of water vapor (H₂O), carbon dioxide (CO₂), and other practical operational considerations. The analysis encompasses their inhibitory and promotional effects on CO-PROX reactions. In addition, we summarize and suggest possible strategies for enhancing CO-PROX tolerance in this work. The catalytic performance can be augmented by modulating the reaction temperature and the feed atmosphere, and catalyst could be activated through pre-treatment with specific atmosphere. High-tolerability CO-PROX catalysts can be developed by meticulously selecting appropriate supports and active-sites. Furthermore, several studies have successfully elevated the reaction performance by integrating insights from other research disciplines. Thereby, this review serves as a valuable reference bridging fundamental research with practical engineering applications within the CO-PROX domain.

Key words: preferential oxidation of CO, H₂O and CO₂ factors, inhibition/promotion effect, regulatory strategy

引用此文

王力鹏, 曹道帆, 刘雪, 李超, 刘科. 工况条件下富氢气体中CO选择性氧化反应的耐受性调控及作用机制研究[J]. 化学学报, 2024, 82(7): 819-832.

Lipeng Wang, Daofan Cao, Xue Liu, Chao Li, Ke Liu. Effect of Realistic Operating Considerations on Preferential Oxidation of CO and Regulatory Strategies: A Review and Perspectives[J]. Acta Chimica Sinica, 2024, 82(7): 819-832.

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图/表 5

图1. CO和H2在CuO-CeO2催化剂上的反应模型

Figure 1. Reaction model of CO and H2 oxidation over CuO-CeO2 catalyst

图2. 双功能催化剂体系上H2O和H2参与的低温PROX反应过程, 以Ni-MgO、FeOx和Fe-Al2O3负载Pt的催化剂为例

Figure 2. Low temperature PROX reaction by dual-functional catalysis in the presence of H2O (H2) on Pt supported with Ni-MgO, FeOx, or Fe-Al2O3

图3. Ru@Pt催化体系通过H*辅助O2解离进而催化PROX的反应过程

Figure 3. The elementary steps for PROX via the H* assisted O2 dissociation over Ru@Pt catalyst

图4. 以最大CO转化率和对应温度窗口划分的不同类型PROX催化剂性能概念图[9]

Figure 4. Conceptual illustration of catalytic performances of different types of catalysts for PROX reaction (the maximum CO conversion and reaction temperature window)[9]

图5. (a)实验室条件下的两级CO-PROX反应单元工艺设计示意图[57], (b)对比单级和双级CO-PROX反应器单元在进料流中不含CO2和H2O的情况下的反应活性[59]

Figure 5. (a) Schematic of double-stage process for the preferential CO oxidation reaction[57], (b) comparison of the overall activity of the single- and double-stage processes without CO2 and H2O in the feed stream[59]

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工况条件下富氢气体中CO选择性氧化反应的耐受性调控及作用机制研究

Effect of Realistic Operating Considerations on Preferential Oxidation of CO and Regulatory Strategies: A Review and Perspectives

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