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由生物质衍生的 N 掺杂蜂窝状多孔碳作为 HS 选择氧化的高效碳催化剂。

N-doped honeycomb-like porous carbon derived from biomass as an efficient carbocatalyst for HS selective oxidation.

机构信息

School of Chemical Engineering, Sichuan University, Chengdu, 610065, China; Dalian National Laboratory for Clean Energy (DNL), Dalian Institute of Chemical Physics, Chinese Academy of Science, 457 Zhongshan Road, Dalian, 116023, China.

State Key Laboratory of Industrial Vent Gas Reuse, Southwest Research & Design Institute of Chemical Industry Co., Ltd. 393 Jindu Section, Airport Road, Chengdu, 610225, China.

出版信息

J Hazard Mater. 2021 Feb 5;403:123806. doi: 10.1016/j.jhazmat.2020.123806. Epub 2020 Sep 3.

DOI:10.1016/j.jhazmat.2020.123806
PMID:33264908
Abstract

3D interconnected porous N-doped carbocatalyst derived from the waste air-laid paper plays as an efficient metal-free catalyst for HS removal in super-Claus reaction. The honeycomb-like porous nitrogen-doped carbons are fabricated through a facile impregnation of alkaline solution and NH post-treatment method. The experiments prove that NH post-treatment is an efficient way to improve the catalytic performance, which resulting in outstanding reactivity and stability with highest sulfur formation rate of 496.6 gkg h and sulfur yield of 86.7 % in feed gas with high concentration (ca. 10,000 ppm) of HS for selective oxidation. Significantly, the optimized pyridinic-N content and defect degree endow the N-doped porous carbon (NPC700) with highest catalytic activity according to the Raman and XPS results. The high surface area and abundant porous structure also contribute to the high catalytic performance by increasing the exposure degree of active site and offering additional active surface. Based on the XPS, SEM, TEM and EDS mapping results, the N-doped porous carbon are proved to be stable catalysts since the morphology and surface chemical environment remain similar after the oxidative desulfurization process.

摘要

由废弃空气铺设纸衍生的 3D 互联多孔 N 掺杂碳催化剂在超级 Claus 反应中用作高效无金属 HS 去除的金属催化剂。通过简单的浸渍碱性溶液和 NH 后处理方法制备了蜂窝状多孔氮掺杂碳。实验证明,NH 后处理是一种提高催化性能的有效方法,从而在高浓度(约 10000ppm)HS 的进料气中具有出色的反应性和稳定性,选择性氧化的最高硫形成速率为 496.6gkg h,硫收率为 86.7%。值得注意的是,优化的吡啶-N 含量和缺陷程度根据拉曼和 XPS 结果赋予 N 掺杂多孔碳(NPC700)最高的催化活性。高比表面积和丰富的多孔结构也通过增加活性位点的暴露程度和提供额外的活性表面来提高催化性能。根据 XPS、SEM、TEM 和 EDS 映射结果,N 掺杂多孔碳被证明是稳定的催化剂,因为氧化脱硫过程后其形态和表面化学环境保持相似。

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