A General Dual-Metal Nanocrystal Dissociation Strategy to Generate Robust High-Temperature-Stable Alumina-Supported Single-Atom Catalysts.
A General Dual-Metal Nanocrystal Dissociation Strategy to Generate Robust High-Temperature-Stable Alumina-Supported Single-Atom Catalysts.
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用于生成鲁棒高温稳定氧化铝支撑单原子催化剂的通用双金属纳米晶体解离策略。
DOI：
10.1021/jacs.3c02909
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发表时间：
2023-07
影响因子：
15
通讯作者：
Zhiquan Hou;Yue Lu;Yuxi Liu;N. Liu;Jingcong Hu;Lu Wei;Zeya Li;X. Tian;Ruyi Gao;Xiaohui Yu;Yuan Feng;Linke Wu;Jiguang Deng;Dingsheng Wang;Manling Sui;H. Dai;Yadong Li
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文献类型：
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作者：
Zhiquan Hou;Yue Lu;Yuxi Liu;N. Liu;Jingcong Hu;Lu Wei;Zeya Li;X. Tian;Ruyi Gao;Xiaohui Yu;Yuan Feng;Linke Wu;Jiguang Deng;Dingsheng Wang;Manling Sui;H. Dai;Yadong Li
设计新的合成路线来制备高耐热贵金属单原子催化剂(SACS)在工业应用中具有挑战性。本文提出了一种从双金属纳米晶(NCS)出发，以双金属纳米晶为促进剂，将一系列贵金属自发转化为氧化铝表面单原子的一般策略。金属单原子被形成在反尖晶石(AB2O4)结构表面的原位阳离子缺陷俘获，这一过程提供了大量的锚定位置，从而促进了孤立金属原子的产生，从而有助于实现非凡的热力学稳定性。在苛刻的老化条件下，Pd1/AlCo2O4-Al_2O_3不仅表现出更好的低温活性，而且对CO和丙烷氧化表现出前所未有的(水)热稳定性。此外，我们的策略通过商业金属氧化物聚集体与Al_2O_3的简单物理混合显示了小的放大效应。这些离子钯物种在氧化气氛和还原气氛之间具有良好的再生性，这使得该催化剂系统在排放控制方面具有潜在的兴趣。
Designing new synthesis routes to fabricate highly thermally durable precious metal single-atom catalysts (SACs) is challenging in industrial applications. Herein, a general strategy is presented that starts from dual-metal nanocrystals (NCs), using bimetallic NCs as a facilitator to spontaneously convert a series of noble metals to single atoms on aluminum oxide. The metal single atoms are captured by cation defects in situ formed on the surface of the inverse spinel (AB2O4) structure, which process provides numerous anchoring sites, thus facilitating generation of the isolated metal atoms that contributes to the extraordinary thermodynamic stability. The Pd1/AlCo2O4-Al2O3 shows not only improved low-temperature activity but also unprecedented (hydro)thermal stability for CO and propane oxidation under harsh aging conditions. Furthermore, our strategy exhibits a small scaling-up effect by the simple physical mixing of commercial metal oxide aggregates with Al2O3. The good regeneration between oxidative and reductive atmospheres of these ionic palladium species makes this catalyst system of potential interest for emissions control.