N-doped honeycomb-like porous carbon derived from biomass as an efficient carbocatalyst for H2S selective oxidation

被引:82
作者
Xu, Chi [1 ,2 ]
Chen, Jian [3 ]
Li, Shiyan [2 ]
Gu, Qingqing [2 ]
Wang, Dajun [3 ]
Jiang, Chengfa [1 ]
Liu, Yuefeng [2 ]
机构
[1] Sichuan Univ, Sch Chem Engn, Chengdu 610065, Peoples R China
[2] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy DNL, 457 Zhongshan Rd, Dalian 116023, Peoples R China
[3] Southwest Res & Design Inst Chem Ind Co Ltd, State Key Lab Ind Vent Gas Reuse, 393 Jindu Sect,Airport Rd, Chengdu 610225, Peoples R China
基金
中国国家自然科学基金;
关键词
Selective oxidation of H2S; Biomass-derived carbon; Nitrogen-doped carbon materials; 3D honeycomb structure; Desulfurization; METAL-FREE CATALYST; FREE ELECTROCATALYSTS; HYDROGEN-SULFIDE; ACTIVATED CARBON; HIGHLY EFFICIENT; NITROGEN; NANOTUBES; OXYGEN; PERFORMANCE; SPHERES;
D O I
10.1016/j.jhazmat.2020.123806
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
3D interconnected porous N-doped carbocatalyst derived from the waste air-laid paper plays as an efficient metal-free catalyst for H2S removal in super-Claus reaction. The honeycomb-like porous nitrogen-doped carbons are fabricated through a facile impregnation of alkaline solution and NH3 post-treatment method. The experiments prove that NH3 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 g(sulfur)kg(cat)(-1) h(-1) and sulfur yield of 86.7 % in feed gas with high concentration (ca. 10,000 ppm) of H2S 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.
引用
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页数:10
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