双金属片
催化作用
亚硝酸盐
密度泛函理论
化学
反应性(心理学)
金属
硝酸盐
选择性
纳米颗粒
单层
选择性催化还原
合理设计
无机化学
化学工程
纳米技术
计算化学
材料科学
有机化学
病理
工程类
医学
替代医学
生物化学
作者
Hao Li,Sujin Guo,Kihyun Shin,Michael S. Wong,Graeme Henkelman
标识
DOI:10.1021/acscatal.9b02182
摘要
Nitrate (NO3–) is a ubiquitous contaminant in groundwater that causes serious public health issues around the world. Though various strategies are able to reduce NO3– to nitrite (NO2–), a rational catalyst design strategy for NO2– removal has not been found, in part because of the complicated reaction network of nitrate chemistry. In this study, we show, through catalytic modeling with density functional theory (DFT) calculations, that the performance of mono- and bimetallic surfaces for nitrite reduction can be rapidly screened using N, N2, and NH3 binding energies as reactivity descriptors. With a number of active surface atomic ensembles identified for nitrite reduction, we have designed a series of “metal-on-metal” bimetallics with optimized surface reactivity and a maximum number of active sites. Choosing Pd-on-Au nanoparticles (NPs) as candidate catalysts, both theory and experiment find that a thin monolayer of Pd-on-Au NPs (size: ∼4 nm) leads to high nitrite reduction performance, outperforming pure Pd NPs and the other Pd surface compositions considered. Experiments show that this thin layer of Pd-on-Au has a relatively high selectivity for N2 formation, compared to pure Pd NPs. More importantly, our study shows that a simple model, based upon DFT-calculated thermodynamic energies, can facilitate catalysts design relevant to environmental issues.
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