纳米材料基催化剂
一氧化碳中毒
催化作用
铂金
一氧化碳
化学
吸附
贵金属
光化学
纳米技术
材料科学
物理化学
有机化学
作者
Wenyao Chen,Jianting Cao,Wenzhao Fu,Jing Zhang,Gang Qian,Jia Yang,De Chen,Xinggui Zhou,Yuan Wang,Xuezhi Duan
标识
DOI:10.1002/anie.202200190
摘要
Carbon monoxide (CO) is notorious for its strong adsorption to poison platinum group metal catalysts in the chemical industry. Here, we conceptually distinguish and quantify the effects of the occupancy and energy of d electrons, emerging as the two vital factors in d-band theory, for CO poisoning of Pt nanocatalysts. The stepwise defunctionalization of carbon support is adopted to fine-tune the 5d electronic structure of supported Pt nanoparticles. Excluding other promotional mechanisms, the increase of Pt 5d band energy strengthens the competitive adsorption of hydrogen against CO for the preferential oxidation of CO, affording the scaling relationship between Pt 5d band energy and CO/H2 adsorption energy difference. The decrease of Pt 5d band occupancy lowers CO site coverage to promote its association with oxygen for the total oxidation of CO, giving the scaling relationship between Pt 5d occupancy and activation energy. The above insights outline a molecular-level understanding of CO poisoning.
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