Abstract Unraveling the structural and kinetic consequences of catalyst properties, which vary with the catalyst preparation methods, on their catalytic behaviors is of prime scientific and industrial importance. Exemplified by Pt/CNT-catalyzed hydrolytic dehydrogenation of ammonia borane (AB), this work examines the origin of the crucial impacts of the catalyst reduction methods (i.e., in situ reduction with AB and ex situ reduction with H 2 ) on the surface and electronic properties of the catalyst as well as the consequent hydrogen generation activity and durability. Kinetic and isotopic analyses reveal that the Pt/CNT-ex situ catalyst has low activation energy and a strong ability to activate water. The relationship between the catalyst structure and performance is established, and the unique surface (e.g., fewer Pt O bonds) and electronic properties (e.g., higher Pt binding energy) of the Pt/CNT-ex situ catalyst are deemed to be responsible for the high activity and durability. The insights reported in this work highlight the importance of understanding the preparation-structure-performance relationship to guide the rational design of catalysts.

中文翻译：

---

氨硼烷制氢过程中 Pt/CNT 催化剂的结构和动力学见解

摘要 阐明随催化剂制备方法不同而变化的催化剂性质对其催化行为的结构和动力学影响具有重要的科学和工业意义。以 Pt/CNT 催化的氨硼烷 (AB) 水解脱氢为例，这项工作研究了催化剂还原方法（即用 AB 原位还原和用 H 2 异位还原）对表面和催化剂的电子特性以及随之而来的产氢活性和耐久性。动力学和同位素分析表明，Pt/CNT-ex situ 催化剂具有低活化能和很强的活化水能力。建立了催化剂结构和性能之间的关系，以及独特的表面（例如，Pt/CNT-ex situ 催化剂的更少 Pt O 键）和电子特性（例如，更高的 Pt 结合能）被认为是高活性和耐久性的原因。这项工作中报告的见解强调了理解制备-结构-性能关系以指导催化剂合理设计的重要性。