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通过惰性纳米覆盖层屏蔽铂/γ-氮化钼可实现稳定的氢气生成。

Shielding Pt/γ-MoN by inert nano-overlays enables stable H production.

作者信息

Gao Zirui, Li Aowen, Liu Xingwu, Peng Mi, Yu Shixiang, Wang Maolin, Ge Yuzhen, Li Chengyu, Wang Tie, Wang Zhaohua, Zhou Wu, Ma Ding

机构信息

Beijing National Laboratory for Molecular Sciences, New Cornerstone Science Laboratory, College of Chemistry and Molecular Engineering, Peking University, Beijing, China.

School of Physical Sciences, University of Chinese Academy of Sciences, Beijing, China.

出版信息

Nature. 2025 Feb;638(8051):690-696. doi: 10.1038/s41586-024-08483-w. Epub 2025 Feb 12.

Abstract

The use of reactive supports to disperse metal species is crucial for constructing highly efficient interfacial catalysts, by tuning the competitive reactant adsorption-activation pattern in supported metal catalysts into a non-competitive mechanism. However, these reactive supports are prone to deterioration during catalysis, limiting the lifespan of the catalyst and their potential practical applications. New strategies are needed to simultaneously protect reactive supports and surface metal species without compromising the inherent catalytic performance. Here we report a new strategy to augment the structural stability of highly active interfacial catalysts by using inert nano-overlays to partially shield and partition the surface of the reactive support. Specifically, we demonstrate that atomically dispersed inert oxide nano-overlays on a highly active Pt/γ-MoN catalyst can block the redundant surface sites of γ-MoN responsible for surface oxidation of this reactive support and the resulting deactivation. This strategy yields an efficient and highly durable catalyst for hydrogen production by methanol-reforming reaction with a mere 0.26 wt% Pt loading, exhibiting a record-high turnover number, to our knowledge, of 15,300,000 and a notable apparent turnover frequency of . This innovative approach showcases the prospects of reducing noble metal consumption and boosting longevity, which could be applied to design effective and stable heterogeneous catalysts.

摘要

通过将负载型金属催化剂中竞争性的反应物吸附 - 活化模式调整为非竞争性机制,使用活性载体来分散金属物种对于构建高效界面催化剂至关重要。然而,这些活性载体在催化过程中容易劣化,限制了催化剂的寿命及其潜在的实际应用。需要新的策略来同时保护活性载体和表面金属物种,而不损害其固有的催化性能。在此,我们报告一种新策略,即通过使用惰性纳米覆盖层部分屏蔽和分隔活性载体表面,增强高活性界面催化剂的结构稳定性。具体而言,我们证明在高活性Pt/γ - MoN催化剂上原子分散的惰性氧化物纳米覆盖层可以阻断γ - MoN上导致该活性载体表面氧化及失活的多余表面位点。该策略通过甲醇重整反应制备了一种高效且高度耐用的制氢催化剂,仅负载0.26 wt%的Pt,据我们所知,其周转数高达15300000,表观周转频率显著。这种创新方法展示了减少贵金属消耗和提高催化剂寿命的前景,可应用于设计有效且稳定的多相催化剂。

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