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Developing a suitable catalyst for the elimination of highly toxic carbonyl sulfide (COS) and hydrogen sulfide (H2S) is of great significance in terms of industrial safety and environmental protection. We demonstrate here the facile synthesis of graphitized 2D micro-meso-macroporous carbons by one-step carbonization of a mixture of urea and glucose at 700-900 degrees C. The as-synthesized graphitized catalysts, designated as 2DNHPC-x (x = urea/glucose mass ratio), are endowed with an ultra-high concentration (12.9-20.2 wt%) of stable and versatile nitrogen sites (e.g. pyrrole and pyridine) which are anchored on the surface via stable covalent bonding. As a result, the 2D-NHPC-x are active in catalytic hydrolysis of COS on pyrrolic N to H2S, and the H2S can be subsequently captured on pyridinic N and converted to elemental sulfur at ambient conditions over the same materials. Among the prepared catalysts, 2D-NHPC-x can catalytically hydrolysize 91% of COS to H2S at 30 degrees C, whereas the conversion ratio over the common catalysts g-C3N4 and Fe2O3 are below 6.0%. Furthermore, these catalysts also exhibit H2S conversion and sulfur selectivity of nearly 100% at 180 degrees C with long-time durability, which is higher than those of the most reported carbonbased catalysts. In contrast, the H2S capacities of activated carbon, ordered mesoporous carbons (OMC) and N-doped OMC are 3.9, 1.5 and 2.39 mmol g-1, respectively. Both the experimental and theoretical results are disclosed that 2D-NHPC-x are superior to the nitrogen-doped porous materials ever applied in simultaneous catalytic elimination of both COS and H2S. (c) 2020 Institute of Process Engineering, Chinese Academy of Sciences. Publishing services by Elsevier B.V. on behalf of KeAi Communications Co., Ltd. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
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GREEN ENERGY & ENVIRONMENT
ISSN: 2096-2797
CN: 10-1418/TK
Year: 2022
Issue: 5
Volume: 7
Page: 983-995
1 3 . 3
JCR@2022
1 0 . 7 0 0
JCR@2023
ESI Discipline: ENGINEERING;
ESI HC Threshold:66
JCR Journal Grade:1
CAS Journal Grade:1
Cited Count:
WoS CC Cited Count: 38
SCOPUS Cited Count:
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 1
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