钴助贵金属催化剂用于氨硼烷水解高效制氢,Journal of the American Chemical Society

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钴助贵金属催化剂用于氨硼烷水解高效制氢
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-02-23 , DOI: 10.1021/jacs.3c00047
Yali Meng ₁ , Qinghao Sun ₁ , Tianjun Zhang ₂ , Jichao Zhang ₃ , Zhuoya Dong ₄ , Yanhang Ma ₄ , Zhangxiong Wu ₅ , Huifang Wang ₆ , Xiaoguang Bao _{1,

7} , Qiming Sun _{1,

7} , Jihong Yu _{1,

2}

Affiliation

Innovation Center for Chemical Sciences, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, People's Republic of China.
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry; International Center of Future Science, Jilin University, Changchun 130012, People's Republic of China.
Shanghai Synchrotron Radiation Facility, Zhangjiang Lab, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201204, People's Republic of China.
School of Physical Science and Technology & Shanghai Key Laboratory of High-resolution Electron Microscopy, ShanghaiTech University, Shanghai 201210, People's Republic of China.
Particle Engineering Laboratory, School of Chemical and Environmental Engineering, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou 215123, People's Republic of China.
Department of Chemistry, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, No. 199, Ren-Ai Road, Suzhou Industrial Park, Suzhou 215123, People's Republic of China.
Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou 215123, People's Republic of China.

氨硼烷（AB）被认为是一种很有前途的化学储氢材料。然而，开发高效、低成本和稳定的AB水解生成H ₂催化剂仍然是实现其实际应用的瓶颈。在此，已经开发了逐步还原策略以在各种金属氧化物载体上合成一系列具有小尺寸和高分散性的双金属物种。优于其他非贵金属物种，Co 物种的引入可以显着和普遍地促进各种贵金属（例如，Pt、Rh、Ru 和 Pd）在 AB 水解反应中的催化活性。优化的Pt _0.1% Co _3% /TiO ₂催化剂表现出超高的H ₂AB 水解的生成率，显示转换频率 (TOF) 值为 2250 mol _{H ₂} mol _Pt^–1 min ^–1在 298 K。这样的 TOF 值比单金属 Pt/TiO ₂高约 10 和 15 倍和商用 Pt/C 催化剂。密度泛函理论（DFT）计算表明，Pt和CoO物种之间的协同作用可以显着促进水分子的化学吸附和解离，加速AB水解产生的H _{2 。}值得注意的是，具有代表性的 Pt _0.25% Co _3% /TiO ₂催化剂表现出优异的稳定性，在室温下实现了高达 215,236 的历史最高周转数。所设计催化剂优异的催化性能、稳定性和低成本为其在化学储氢中的实际应用开辟了新的前景。

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Cobalt-Promoted Noble-Metal Catalysts for Efficient Hydrogen Generation from Ammonia Borane Hydrolysis

Ammonia borane (AB) has been regarded as a promising material for chemical hydrogen storage. However, the development of efficient, cost-effective, and stable catalysts for H₂ generation from AB hydrolysis remains a bottleneck for realizing its practical application. Herein, a step-by-step reduction strategy has been developed to synthesize a series of bimetallic species with small sizes and high dispersions onto various metal oxide supports. Superior to other non-noble metal species, the introduction of Co species can remarkably and universally promote the catalytic activity of various noble metals (e.g., Pt, Rh, Ru, and Pd) in AB hydrolysis reactions. The optimized Pt_0.1%Co_3%/TiO₂ catalyst exhibits a superhigh H₂ generation rate from AB hydrolysis, showing a turnover frequency (TOF) value of 2250 mol_H₂ mol_Pt^–1 min^–1 at 298 K. Such a TOF value is about 10 and 15 times higher than that of the monometal Pt/TiO₂ and commercial Pt/C catalysts, respectively. The density functional theory (DFT) calculation reveals that the synergy between Pt and CoO species can remarkably promote the chemisorption and dissociation of water molecules, accelerating the H₂ evolution from AB hydrolysis. Significantly, the representative Pt_0.25%Co_3%/TiO₂ catalyst exhibits excellent stability, achieving a record-high turnover number of up to 215,236 at room temperature. The excellent catalytic performance, superior stability, and low cost of the designed catalysts create new prospects for their practical application in chemical hydrogen storage.

更新日期：2023-02-23

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