Highly stable and active catalysts are of significant importance and a longstanding challenge for a number of industrial chemical transformations. Here, motivated by the principle of the high entropy-stabilized structure, high-entropy alloy-loaded porous TiO₂ as an efficient and sintering-resistant catalyst for the light-driven reverse water gas‒shift reaction without external heating is synthesized. The optimized CoNiCuPdRu/TiO₂ catalyst exhibits a long-term stability of 1000 h (1.23 mol g_metal ⁻¹ h⁻¹ CO production rate, >99% high selectivity). In situ characterizations confirm that the slow diffusion effect of high-entropy alloys endows the catalyst with excellent structural stability. The CO adsorption measurements and theoretical calculations consolidate that the hydrogen surface coverage weakens CO adsorption on the catalyst surface. Two major problems of catalyst deactivation − sintering and poisoning, are handled in one case, which synergistically enable unparalleled stability. This work provides new guidance for the rational design of ultradurable harsh-condition operation catalysts for industrial catalysis.

中文翻译：

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对高熵合金催化剂具有 1000 h 稳定性的轻驱动反水煤气变换反应


高度稳定和活性的催化剂具有重要意义，也是许多工业化学转化面临的长期挑战。在这里，在高熵稳定结构原理的推动下，合成了高熵负载合金的多孔 TiO₂ 作为一种高效且耐烧结的催化剂，用于无需外部加热的光驱动反向水气-转移反应。优化的 CoNiCuPdRu/TiO₂ 催化剂表现出 1000 h 的长期稳定性（1.23 mol g_金属⁻¹ h⁻¹ CO产生速率，>99% 高选择性）。原位表征证实，高熵合金的缓慢扩散效应赋予了催化剂优异的结构稳定性。CO 吸附测量和理论计算证实，氢表面覆盖削弱了 CO 在催化剂表面的吸附。催化剂失活的两个主要问题 - 烧结和中毒，在一个案例中得到处理，它们协同作用，实现了无与伦比的稳定性。这项工作为工业催化用超耐用恶劣条件操作催化剂的合理设计提供了新的指导。