氢氧化铁负载亚纳米铂族金属催化剂室温湿氧化消除CO

doi:10.1016/S1872-2067(19)63489-3

催化学报 ›› 2020, Vol. 41 ›› Issue (4): 613-621.DOI: 10.1016/S1872-2067(19)63489-3

• 中国科学院青年创新促进会专栏 • 上一篇下一篇

氢氧化铁负载亚纳米铂族金属催化剂室温湿氧化消除CO

关红玲^a, 陈洋^b, 阮崇焱^b, 林坚^b, 苏杨^b, 王晓东^b, 屈凌波^c

a 郑州大学化工学院, 河南郑州 450001;
b 中国科学院大连化学物理研究所, 中国科学院航天催化材料重点实验室, 辽宁大连 116023;
c 郑州大学化学学院, 河南郑州 450001

收稿日期:2019-08-30 修回日期:2019-09-27 出版日期:2020-04-18 发布日期:2019-12-12
通讯作者: 林坚, 王晓东
基金资助:
国家自然科学基金（21576251，21676269，21808212，21878283）；中国科学院青年创新促进会（2017223）；国家重点研发计划（2016YFA0202801）；中国科学院战略性先导科技专项（XDB17020100）；国家博士后自然基金（2019M652578）；河南省博士后科研启动项目（1902015）；河南省科技攻关项目（192102210034）；中原博士后创新人才支持计划.

Versatile application of wet-oxidation for ambient CO abatement over Fe(OH)_x supported subnanometer platinum group metal catalysts

Hongling Guan^a, Yang Chen^b, Chongyan Ruan^b, Jian Lin^b, Yang Su^b, Xiaodong Wang^b, Lingbo Qu^c

a School of Chemical Engineering, Zhengzhou University, Zhengzhou 450001, Henan, China;
b CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
c College of Chemistry, Zhengzhou University, Zhengzhou 450001, Henan, China

Received:2019-08-30 Revised:2019-09-27 Online:2020-04-18 Published:2019-12-12
Supported by:
This work was supported by the National Natural Science Foundation of China (21576251, 21676269, 21808212, 21878283), the Youth Innovation Promotion Association CAS (2017223), National Key Projects for Fundamental Research and Development of China (2016YFA0202801), the "Strategic Priority Research Program" of the Chinese Academy of Sciences (XDB17020100), China Postdoctoral Science Foundation (2019M652578), the Postdoctoral Sponsorship in Henan Province (1902015), Science and Technology Program of Henan Province (192102210034), and Zhongyuan Postdoctoral Program for Innovation Talents.

摘要/Abstract

摘要： 室温条件下高效消除CO具有重要的意义，但目前仍具有极大的挑战.考虑到实际应用环境中存在的水汽，实现具有应用价值的CO消除过程的关键是设计耐湿性好，且能够在室温甚至更低温度下具有较高CO氧化活性的催化剂.以Hopcalite （Cu-Mn-O_x）和Co₃O₄为代表的氧化物和负载型Au基催化剂具有优异的低温CO氧化活性，但存在耐湿性差、催化性能重复性不好等缺点，因而限制了其实际应用.铂族金属催化剂凭借优异的稳定性和耐湿性成为目前最广泛应用的尾气净化催化剂.但是由于铂金属位点强吸附CO的毒化作用，CO氧化工作温度多在200℃以上，从而限制了其在室内空气净化、燃料电池工业氢源净化以及汽车发动机冷启动阶段尾气净化等过程中的实际应用.研究人员尝试调节金属粒子尺寸、金属-载体界面、双金属结构及助剂效应等以促进O₂的活化或者削弱CO的吸附，尽管取得了一定的进展，但仍缺少一种具有普适性和实际CO消除应用前景的铂族金属基催化体系.本文利用新型Fe(OH）_x负载亚纳米Rh催化剂作为室温条件下CO湿氧化的典型例子，研究H₂O对CO氧化反应的影响并探索其反应机制，旨在为发展实际可用的CO氧化消除催化体系提供参考.
活性测试结果表明，H₂O的存在可以大幅提高Fe(OH）_x负载亚纳米Rh催化剂的CO氧化速率，并在室温条件下实现CO的长效稳定消除；而相似共沉淀法制备的Rh/Al₂O₃催化剂上H₂O并没有促进CO氧化.原位红外表征发现，Fe(OH）_x在湿氧化CO过程中的重要作用在于为O₂和H₂O的吸附提供位点，促进二者反应生成羟基物种，并与亚纳米Rh团簇上吸附的CO反应生成CO₂.此外，H₂O的存在使得CO氧化的表观活化能由22降至9kJ mol^-1，说明反应路径或决速步骤由CO+O转变为反应能垒更低的CO+OH，从而大幅提高了CO氧化反应速率和反应活性.随后，时间分辨CO滴定红外实验证明，Rh/Fe(OH）_x催化剂表面OH可以与CO反应生成CO₂，而Al₂O₃负载的纳米Rh催化剂则不能，从而进一步揭示了Fe(OH）_x载体在高效湿氧化消除CO过程中的重要作用.最后，通过拓展实验证明该反应机理可以适用于Fe(OH）_x负载的其它铂族金属催化剂，提供了一种具有普适性和实际CO消除应用前景的铂族金属基催化体系.

关键词: 铂族金属, 一氧化碳, 氧化, 室温条件, Fe(OH)_x, 亚纳米团簇

Abstract: The efficient and stable abatement of CO pollutant under ambient conditions is of great significance; however, it remains a formidable challenge. Herein, we report the versatile application of wet oxidation over Fe(OH)_x supported subnanometer Pt group metal (PGM) catalysts for the complete removal of CO under ambient temperature and humidity conditions. Typically, the 1.8 wt% Rh/Fe(OH)_x catalyst exhibited better durability during a~1400 min run for wet oxidation than for dry CO oxidation. Multiple characterization results including HR-TEM, H₂-TPR, and in-situ DRIFTS suggested that Fe(OH)_x, with good reducibility, promoted by the subnanometer Rh clusters, provided sites for the adsorption and reaction of O₂ and H₂O to form OH species. Subsequently, these OH species reacted with the adsorbed CO on Rh sites with a considerably lower activation energy (9 kJ mol^-1) than that of dissociated O species (22 kJ mol^-1), thus rationalizing the outstanding performance of Rh/Fe(OH)_x for wet oxidation. Extended experiments with other PGMs revealed a good generality for the application of wet oxidation in the efficient abatement of CO under humid conditions with Fe(OH)_x as the support.

Key words: Platinum group metals, CO, Oxidation, Ambient condition, Fe(OH)_x, Subnanometer clusters

关红玲, 陈洋, 阮崇焱, 林坚, 苏杨, 王晓东, 屈凌波. 氢氧化铁负载亚纳米铂族金属催化剂室温湿氧化消除CO[J]. 催化学报, 2020, 41(4): 613-621.

Hongling Guan, Yang Chen, Chongyan Ruan, Jian Lin, Yang Su, Xiaodong Wang, Lingbo Qu. Versatile application of wet-oxidation for ambient CO abatement over Fe(OH)_x supported subnanometer platinum group metal catalysts[J]. Chinese Journal of Catalysis, 2020, 41(4): 613-621.

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氢氧化铁负载亚纳米铂族金属催化剂室温湿氧化消除CO

Versatile application of wet-oxidation for ambient CO abatement over Fe(OH)_x supported subnanometer platinum group metal catalysts

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氢氧化铁负载亚纳米铂族金属催化剂室温湿氧化消除CO

Versatile application of wet-oxidation for ambient CO abatement over Fe(OH)x supported subnanometer platinum group metal catalysts

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Versatile application of wet-oxidation for ambient CO abatement over Fe(OH)_x supported subnanometer platinum group metal catalysts