Pt-Based Carbon Fiber Catalytic Dehydrogenation of Methylcyclohexane in a Fixed-Bed Reactor

IF 5.3 3区 工程技术 Q2 ENERGY & FUELS
Wei Chen, Zhao Zhang*, Yueer Ma, Xiaomin Dai, Ruixin Wang, Yangyi Chen, Chuanyin Xiong, Yuxia Luo, Xinping Li and Hui Chang*, 
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Abstract

In this study, carbon fibers (CF) were modified by gas-phase (G), liquid-phase (L), and gas–liquid-phase (GL) oxidation methods, on which the platinum (Pt) was further loaded to prepare catalysts of Pt/CF-G, Pt/CF-L, and Pt/CF-GL, respectively. The fluffy stacking of one-dimensional fibrous catalysts endowed Pt/CF-G, Pt/CF-L, and Pt/CF-GL with excellent mass transfer efficiency, enabling them to self-support and directly be used in a fixed bed. Compared with primary CF, the oxygen content on the surface of CF-GL increased by 75.2%. The increase in the oxygen-containing groups on the surface of CF-GL not only facilitated the Pt atoms anchoring (enhancing the Pt loading from 1.76 to 2.44%) but also effectively improved the dispersion of Pt particles (reducing the Pt nanoparticle size from 4.68 to 3.73 nm). The catalyst Pt/CF-GL had the high catalytic activity and achieved the conversion rate of 96.9% during the methylcyclohexane (MCH) dehydrogenation reaction process (28.9, 47.0, and 76.1% for the Pt/CF, Pt/CF-L, and Pt/CF-G catalyst, respectively). Moreover, the catalyst Pt/CF-GL exhibited excellent activity stability after 72 h of continuous MCH dehydrogenation reaction, with a very low inactivation rate (<5%). Obviously, the self-supporting Pt/CF-GL catalyst could be directly used for efficient and stable dehydrogenation of liquid organic hydrogen carriers.

Abstract Image

pt基碳纤维在固定床反应器中催化甲基环己烷脱氢
本研究通过气相(G)、液相(L)和气液相(GL)氧化法对碳纤维(CF)进行改性,在此基础上进一步负载铂(Pt),分别制备了Pt/CF-G、Pt/CF-L和Pt/CF-GL催化剂。一维纤维催化剂的蓬松堆积使Pt/CF-G、Pt/CF-L和Pt/CF-GL具有优异的传质效率,使其能够自支撑并直接在固定床上使用。与原生CF相比,CF- gl表面氧含量提高了75.2%。CF-GL表面含氧基团的增加不仅促进了Pt原子的锚定(将Pt负载从1.76提高到2.44%),而且有效地改善了Pt粒子的分散性(将Pt纳米粒子的尺寸从4.68 nm减小到3.73 nm)。Pt/CF- gl催化剂具有较高的催化活性,在甲基环己烷(MCH)脱氢反应过程中转化率达到96.9% (Pt/CF、Pt/CF- l和Pt/CF- g催化剂分别为28.9%、47.0%和76.1%)。Pt/CF-GL催化剂在连续MCH脱氢72 h后表现出良好的活性稳定性,失活率极低(5%)。显然,自支撑Pt/CF-GL催化剂可直接用于高效、稳定的液态有机氢载体脱氢。
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来源期刊
Energy & Fuels
Energy & Fuels 工程技术-工程:化工
CiteScore
9.20
自引率
13.20%
发文量
1101
审稿时长
2.1 months
期刊介绍: Energy & Fuels publishes reports of research in the technical area defined by the intersection of the disciplines of chemistry and chemical engineering and the application domain of non-nuclear energy and fuels. This includes research directed at the formation of, exploration for, and production of fossil fuels and biomass; the properties and structure or molecular composition of both raw fuels and refined products; the chemistry involved in the processing and utilization of fuels; fuel cells and their applications; and the analytical and instrumental techniques used in investigations of the foregoing areas.
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