Yan Han, Lei Haofan, Qin Xuetao, Liu Jin-Cheng, Cai Lihua, Hu Sunpei, Xiao Zizhen, Peng Fenglin, Wang Wei-Wei, Jin Zhao, Yi Xianfeng, Zheng Anmin, Ma Chao, Jia Chun-Jiang, Zeng Jie
Hefei National Research Center for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
Key Laboratory for Colloid and Interface Chemistry, Key Laboratory of Special Aggregated Materials, School of Chemistry and Chemical Engineering, Shandong University, Jinan, 250100, P. R. China.
Angew Chem Int Ed Engl. 2024 Dec 9;63(50):e202411264. doi: 10.1002/anie.202411264. Epub 2024 Oct 16.
The surface chemistry of CeO is dictated by the well-defined facets, which exert great influence on the supported metal species and the catalytic performance. Here we report Pt/CeO catalysts exhibiting specific structures of Pt-O coordination on different facets by using adequate preparation methods. The simple impregnation method results in Pt-O coordination on the predominantly exposed {111} facets, while the photo-deposition method achieves oriented atomic deposition for Pt-O coordination into the "nano-pocket" structure of {100} facets at the top. Compared to the impregnated Pt/CeO catalyst showing normal redox properties and low-temperature activity for CO oxidation, the photo-deposited Pt/CeO exhibits uncustomary strong metal-support interaction and extraordinary high-temperature stability. The preparation methods dictate the facet-dependent diversity of Pt-O coordination, resulting in the further activity-selectivity trade-off. By applying specific preparation routes, our work provides an example of disentangling the effects of support facets and coordination environments for nano-catalysts.
CeO的表面化学由明确的晶面决定，这些晶面对负载的金属物种和催化性能有很大影响。在此，我们报道了通过使用适当的制备方法，在不同晶面上呈现特定Pt-O配位结构的Pt/CeO催化剂。简单浸渍法导致在主要暴露的{111}晶面上形成Pt-O配位，而光沉积法实现了Pt-O配位的定向原子沉积，形成顶部{100}晶面的“纳米口袋”结构。与表现出正常氧化还原性质和低温CO氧化活性的浸渍型Pt/CeO催化剂相比，光沉积的Pt/CeO表现出异常强的金属-载体相互作用和非凡的高温稳定性。制备方法决定了Pt-O配位的晶面依赖性多样性，导致了进一步的活性-选择性权衡。通过应用特定的制备路线，我们的工作提供了一个解开纳米催化剂载体晶面和配位环境影响的例子。
