K 促进的 Pt/meso-Al2O3 催化剂用于十二氢-N-乙基咔唑脱氢制取 H2

IF 4.1 2区 工程技术 Q2 ENGINEERING, CHEMICAL
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引用次数: 0

摘要

作为一种液态有机氢载体,N-乙基咔唑在储氢技术领域显示出巨大的前景。开发高效稳定的催化剂,通过 N-乙基咔唑脱氢制取氢气,对于其实际应用至关重要。本研究开发了一系列介孔 Al2O3 支持的 K 修饰铂催化剂,用于 N-乙基咔唑脱氢。这些催化剂的表征采用了多种技术,包括 XRD、N2 吸附-解吸、TEM、27Al MAS NMR、XPS、NH3-TPD、H2-TPR、CO-FTIR 和 Py-IR,为阐明结构-活性关系提供了详细的结构信息。研究发现,介孔 Al2O3 中含有大量配位不饱和的五配位 Al3+,这极大地促进了铂物种的分散,从而形成了小的铂颗粒。据观察,K 的加入可调节铂的电子结构、降低催化剂的酸度并抑制铂的烧结。这些协同效应使得 Pt3.0/K3.0-Al2O3-m 在 180 °C 和 101 kPa 条件下的十二氢-N-乙基咔唑脱氢反应中取得了显著的性能,十二氢-N-乙基咔唑转化率达到 100%,H2 释放量达到 5.63 wt%,脱氢效率达到 97.10%。此外,该催化剂在十二氢-N-丙基咔唑、八氢-2-甲基吲哚和八氢-1,2-二甲基吲哚的脱氢过程中也表现出很高的效率,脱氢效率分别达到 99.60%、100% 和 100%。这些发现为合理设计储氢系统中液态有机氢载体的高效金属基催化剂提供了宝贵的知识。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

K-promoted Pt/meso-Al2O3 catalysts for H2 production from dehydrogenation of dodecahydro‑N‑ethylcarbazole

K-promoted Pt/meso-Al2O3 catalysts for H2 production from dehydrogenation of dodecahydro‑N‑ethylcarbazole
N-ethylcarbazole, as a liquid organic hydrogen carrier, has shown great promise in the field of hydrogen storage technology. The development of efficient and stable catalyst for producing H2 through N-ethylcarbazole dehydrogenation is crucial for its practical application. In this study, a series of mesoporous Al2O3-supported Pt catalysts with K modification were developed for N-ethylcarbazole dehydrogenation. These catalysts were characterization using various techniques including XRD, N2 adsorption–desorption, TEM, 27Al MAS NMR, XPS, NH3-TPD, H2-TPR, CO-FTIR, and Py-IR, providing detailed structural information to elucidate the structure–activity relationship. Mesoporous Al2O3 was found to possess significant amounts of coordinatively unsaturated pentacoordinate Al3+, which greatly promotes the dispersion of Pt species for the formation of small Pt particles. The addition of K was observed to modulate the electronic structure of Pt, reduce the acidity of the catalysts, and inhibit the sintering of Pt. These synergetic effects led to Pt3.0/K3.0-Al2O3-m achieving remarkable performance in dodecahydro-N-ethylcarbazole dehydrogenation at 180 °C and 101 kPa, delivering a dodecahydro-N-ethylcarbazole conversion of 100 %, H2 release amount of 5.63 wt% and dehydrogenation efficiency of 97.10 %. Additionally, this catalyst demonstrated high efficiency in the dehydrogenation of dodecahydro-N-propylcarbazole, octahydro-2-methylindole, and octahydro-1,2-dimethylindole, achieving dehydrogenation efficiencies of 99.60 %, 100 % and 100 %, respectively. These findings provide valuable knowledge for the rational design of efficient metal-based catalysts for liquid organic hydrogen carriers in hydrogen storage systems.
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来源期刊
Chemical Engineering Science
Chemical Engineering Science 工程技术-工程:化工
CiteScore
7.50
自引率
8.50%
发文量
1025
审稿时长
50 days
期刊介绍: Chemical engineering enables the transformation of natural resources and energy into useful products for society. It draws on and applies natural sciences, mathematics and economics, and has developed fundamental engineering science that underpins the discipline. Chemical Engineering Science (CES) has been publishing papers on the fundamentals of chemical engineering since 1951. CES is the platform where the most significant advances in the discipline have ever since been published. Chemical Engineering Science has accompanied and sustained chemical engineering through its development into the vibrant and broad scientific discipline it is today.
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