促进十二氢-N-乙基咔唑低温脱氢的锡改性碳支撑钯钴双金属氧化物

IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Fuel Pub Date : 2024-11-15 DOI:10.1016/j.fuel.2024.133718
Wenhua Zhou , Xiaoxuan Li , Chao Chen , Teng Guo , Jianghao Wang , Kaige Wang , Bolong Li , Zhenyu Zhang , Jie Fu
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引用次数: 0

摘要

液态有机氢载体(LOHCs)因其储氢密度高、易于储存和运输而受到广泛关注和研究。研究表明,碳支撑双金属合金作为低温脱氢催化剂表现出卓越的性能。然而,开发高效的碳支撑催化剂并揭示活性金属与支撑物之间的相互作用仍然具有挑战性,但意义重大。在这项工作中,合成了一种具有成本效益的金属改性活性炭(AC),并负载了钯钴氧化物(PdCoO)活性位点,用于十二氢-N-乙基咔唑(12H-NECZ)的低温脱氢制氢。结果表明(1)在 AC 载体中引入锡(Sn)形成高分散的 PdCoO/Sn2-C ,改善了催化剂的孔分布和尺寸,促进了活性金属在表面的分散;(2)PdCoOx 与 Sn-C 载体之间的界面效应有效调节了催化剂内部的电子转移,增强了金属之间的协同效应,降低了电子转移阻力,从而提高了脱氢催化活性。结果表明,在 140 °C 条件下,12H-NECZ 在 8 小时后完全脱氢,选择性达 92.5%,而钯的负载量仅为 2.2 wt%。这项研究为通过改变载体的电子效应有针对性地设计催化剂提供了一种合适的方法。
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Sn modified carbon support PdCo bimetallic oxide for boosting low-temperature dehydrogenation of dodecahydro-N-ethylcarbazole
Liquid organic hydrogen carriers (LOHCs) have garnered considerable attention and have undergone extensive studies owing to their high hydrogen storage density and ease of storage and transportation. Research has shown that carbon-supported bimetallic alloys exhibit exceptional performance as catalysts for low-temperature dehydrogenation. Nevertheless, developing high-efficiency carbon support catalysts and revealing the interaction between active metals and support remains challenging but significant. In this work, a cost-effective metal-modified activated carbon (AC) was synthesized and loaded with PdCoO active sites for low-temperature dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NECZ) to produce hydrogen. The results show that: (1) Introducing tin (Sn) into the AC support to form highly dispersed PdCoO/Sn2-C improves the pore distribution and size of the catalyst, promoting the dispersion of active metals on the surface; (2) The interface effect between PdCoOx and Sn-C supports effectively regulates the electron transfer inside the catalyst, enhances the synergistic effect between metals, and reduces electron transfer resistance, thereby improving dehydrogenation catalytic activity. The results show that at 140 °C, 12H-NECZ was completely dehydrogenated after 8 h, with a selectivity of 92.5%, while the palladium loading was only 2.2 wt%. This study provides a suitable method for the targeted design of catalysts by altering the electronic effects of supports.
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来源期刊
Fuel
Fuel 工程技术-工程:化工
CiteScore
12.80
自引率
20.30%
发文量
3506
审稿时长
64 days
期刊介绍: The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.
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