Continuous and controllable synthesis of MnO2 adsorbents for H2S removal at low temperature

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

doi:10.1016/j.jhazmat.2024.134402

Continuous and controllable synthesis of MnO₂ adsorbents for H₂S removal at low temperature

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

Authors

Chenxiao Zhang¹, Jinyu Zheng², Shikun Su², Ye Jin², Zhuo Chen³, Yundong Wang¹, Jianhong Xu⁴

Affiliations

¹ The State Key Laboratory of Chemical Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China.
² Sinopec Research Institute of Petroleum Processing Co., Ltd, Beijing 102299, China.
³ The State Key Laboratory of Chemical Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China. Electronic address: chenz2022@tsinghua.edu.cn.
⁴ The State Key Laboratory of Chemical Engineering, Department of Chemical Engineering, Tsinghua University, Beijing 100084, China. Electronic address: xujianhong@tsinghua.edu.cn.

PMID: 38688216
DOI: 10.1016/j.jhazmat.2024.134402

Abstract

H₂S is an extremely noxious impurity generated from nature and chemical industrial processes. High performing H₂S adsorbents are required for chemical industry and environmental engineering. Herein, α-, γ-, and δ-MnO₂ 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 H₂S breakthrough tests at 150 °C, continuously prepared α-, γ-, and δ-MnO₂ 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 H₂S adsorption performances.

Keywords: Adsorbent; Continuous synthesis; Crystal phase; H(2)S removal; MnO(2).