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用于低温脱除硫化氢的MnO吸附剂的连续可控合成

Continuous and controllable synthesis of MnO adsorbents for HS removal at low temperature.

作者信息

Zhang Chenxiao, Zheng Jinyu, Su Shikun, Jin Ye, Chen Zhuo, Wang Yundong, Xu Jianhong

机构信息

The State Key Laboratory of Chemical Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China.

Sinopec Research Institute of Petroleum Processing Co., Ltd, Beijing 102299, China.

出版信息

J Hazard Mater. 2024 Jun 5;471:134402. doi: 10.1016/j.jhazmat.2024.134402. Epub 2024 Apr 25.

Abstract

HS is an extremely noxious impurity generated from nature and chemical industrial processes. High performing HS adsorbents are required for chemical industry and environmental engineering. Herein, α-, γ-, and δ-MnO adsorbents with high sulfur capacity were synthesized through a continuous-flow approach with a microreactor system, achieving much higher efficiency than hydrothermal methods. The relationship between crystal structure and synthesis conditions such as residence time, reaction temperature, concentration of K in solution and reactant ratio is discussed. According to the HS breakthrough tests at 150 °C, continuously prepared α-, γ-, and δ-MnO exhibited sulfur capacities of 669.5, 193.8 and 607.6 mg S/g sorbent, respectively, which was at a high level among the reported adsorbents. Such enhanced performance is related to the large surface area and mesopore volume, high reducibility, and a large number of oxygen species with high reactivity and mobility. Manganese sulfide and elemental sulfur were formed after desulfurization, which indicated the reaction consisted of two steps: redox and sulfidation of the sorbents. This study provides an innovative design strategy for the construction of nanomaterials with high HS adsorption performances.

摘要

硫化氢是一种由自然和化学工业过程产生的极具毒性的杂质。化学工业和环境工程需要高性能的硫化氢吸附剂。在此,通过微反应器系统的连续流动方法合成了具有高硫容量的α-、γ-和δ-二氧化锰吸附剂,其效率比水热法高得多。讨论了晶体结构与合成条件(如停留时间、反应温度、溶液中钾的浓度和反应物比例)之间的关系。根据在150°C下的硫化氢穿透试验,连续制备的α-、γ-和δ-二氧化锰的硫容量分别为669.5、193.8和607.6mg S/g吸附剂,在已报道的吸附剂中处于较高水平。这种性能的提高与大表面积和中孔体积、高还原性以及大量具有高反应性和迁移率的氧物种有关。脱硫后形成了硫化锰和元素硫,这表明反应包括两个步骤:吸附剂的氧化还原和硫化。本研究为构建具有高硫化氢吸附性能的纳米材料提供了一种创新的设计策略。

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