Mitigating Hydrogen Poisoning for Robust Ammonia-to-Hydrogen Conversion over Photothermal Catalysts

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-06-04 DOI:10.1021/acscatal.5c0141110.1021/acscatal.5c01411

Jianming Liu, Wangxi Liu, Zhonghua Li, Jun Wang, Rongli Fan, Changhao Liu, Bin Gao*, Zhigang Zou and Zhaosheng Li*,

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Abstract

Ammonia is recognized as a highly promising candidate for hydrogen storage, and its decomposition to hydrogen has attracted increasing attention. Here, photothermal catalysts composed of Ni, Au, or Ru with γ-Al₂O₃ support have been designed for the NH₃-to-H₂ conversion. Ru/γ-Al₂O₃ exhibits the highest NH₃ conversion (84.8%) and H₂ yield (1.7 mol·g_cat^–1·h^–1) at a gas hourly space velocity (GHSV) of 30 L·g_cat^–1·h^–1. H₂ desorption was found to be slower than N₂ desorption over Ru/γ-Al₂O₃ in the dark. The hydrogen poisoning phenomenon was mitigated during the photothermal catalytic process, compared with the thermal catalytic process. Hot carriers generated in the photothermal catalysts were proven to effectively cleave Ru–H* bonds under illumination. Moreover, Ru/γ-Al₂O₃ photothermal catalyst was found to inhibit catalyst aggregation, resulting in robust NH₃-to-H₂ conversion over 1200 h under illumination.

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光热催化剂上稳健氨制氢转化减轻氢中毒

氨被认为是一种极具潜力的储氢材料，其分解制氢引起了越来越多的关注。本文设计了以Ni、Au或Ru为载体，以γ-Al2O3为载体的光热催化剂，用于NH3-to-H2的转化。Ru/γ-Al2O3在气体时空速（GHSV）为30 L·gcat-1·h-1时，NH3转化率最高（84.8%），H2产率最高（1.7 mol·gcat-1·h-1）。在黑暗中，Ru/γ-Al2O3对H2的解吸比N2的解吸慢。与热催化相比，光热催化过程中的氢中毒现象得到了缓解。光热催化剂中产生的热载流子在光照下能有效地裂解Ru-H *键。此外，Ru/γ-Al2O3光热催化剂可以抑制催化剂聚集，在1200 h的光照下，NH3-to-H2的转化率显著提高。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.