通过沸石 13X 负载的 Ni 催化剂分解氨生产清洁氢气,Sustainable Energy & Fuels

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通过沸石 13X 负载的 Ni 催化剂分解氨生产清洁氢气
Sustainable Energy & Fuels ( IF 5.0 ) Pub Date : 2024-01-12 , DOI: 10.1039/d3se01426f
Jiyu Kim _{1,

2} , Kyoung Deok Kim _{1,

3} , Unho Jung ₁ , Yongha Park ₁ , Ki Bong Lee ₂ , Kee Young Koo _{1,

4}

Affiliation

与大多数H _{2生产方法不同，NH}₃的分解不会导致二氧化碳排放，因此被归类为清洁技术。因此，NH _3在H₂的大规模运输和储存方面具有广阔的前景，高效的低温NH ₃分解催化剂备受追捧。在此，我们研究了通过离子交换、沉积沉淀和初湿浸渍制备的13X沸石负载的Ni催化剂的结构性质和NH _{3分解性能。}主要表面物质被确定为 Ni 层状硅酸盐（离子交换）、NiO + Ni 层状硅酸盐（沉积沉淀）和 NiO（浸渍）。与其他催化剂相比，通过沉积沉淀生产的催化剂实现了最高的H ₂形成速率（22.9 mmol g _cat^-1 min ^-1 at 30 000 mL g _cat^-1 h ^-1 , 600 °C），并表现出30–40 °C 降低氮气解吸温度。考虑到氮解吸被认为是催化NH ₃分解的速率决定步骤，解吸温度的降低归因于低温性能的改善。具体来说，通过沉积沉淀获得的催化剂的优异性能归因于活性Ni金属在沸石载体表面和孔道中的高度分散和均匀沉积，其较大的比表面积和较强的金属-载体相互作用。。

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Clean hydrogen production from ammonia decomposition over zeolite 13X-supported Ni catalysts

Unlike most H₂ production methods, the decomposition of NH₃ does not result in carbon dioxide emission and is therefore classified as clean technology. Thus, NH₃ holds great promise for the large-scale transportation and storage of H₂, and efficient low-temperature NH₃ decomposition catalysts are highly sought after. Herein, we examined the textural properties and NH₃ decomposition performances of zeolite 13X-supported Ni catalysts prepared by ion exchange, deposition precipitation, and incipient wetness impregnation. The main surface species were identified as Ni phyllosilicates (ion exchange), NiO + Ni phyllosilicates (deposition precipitation), and NiO (impregnation). Compared to other catalysts, the catalyst produced by deposition precipitation achieved the highest H₂ formation rate (22.9 mmol g_cat⁻¹ min⁻¹ at 30 000 mL g_cat⁻¹ h⁻¹, 600 °C) and exhibited a 30–40 °C lower nitrogen desorption temperature. Given that nitrogen desorption is assumed to be the rate-determining step of catalytic NH₃ decomposition, this decrease in the desorption temperature was attributed to improved low-temperature performance. Specifically, the excellent performance of the catalyst obtained by deposition precipitation was ascribed to its large specific surface area and strong metal-support interactions due to the high dispersion and uniform deposition of the active Ni metal on the surface and in the pores of the zeolite support.

更新日期：2024-01-12

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