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[1]丁晓波,覃远航*.N、S共掺杂碳基高效氧还原催化剂的制备[J].武汉工程大学学报,2021,43(04):362-366.[doi:10.19843/j.cnki.CN42-1779/TQ.202105007]
 DING Xiaobo,QIN Yuanhang*.Preparation of N, S Co-doped Carbon as Highly Efficient Catalyst for Oxygen Reduction[J].Journal of Wuhan Institute of Technology,2021,43(04):362-366.[doi:10.19843/j.cnki.CN42-1779/TQ.202105007]
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《武汉工程大学学报》[ISSN:1674-2869/CN:42-1779/TQ]

卷:
43
期数:
2021年04期
页码:
362-366
栏目:
化学与化学工程
出版日期:
2021-08-31

文章信息/Info

Title:
Preparation of N, S Co-doped Carbon as Highly Efficient Catalyst for Oxygen Reduction
文章编号:
1674 - 2869(2021)04 - 0362 - 05
作者:
丁晓波覃远航*
武汉工程大学化工与制药学院,湖北 武汉 430205
Author(s):
DING Xiaobo QIN Yuanhang*
School of Chemical Engineering and Pharmacy, Wuhan Institute of Technology, Wuhan 430205, China
关键词:
氧还原反应无金属催化剂杂原子掺杂碳石墨相氮化碳
Keywords:
oxygen reduction reaction metal-free catalyst heteroatom-doped carbon graphitic carbon nitride
分类号:
TQ426.7
DOI:
10.19843/j.cnki.CN42-1779/TQ.202105007
文献标志码:
A
摘要:
杂原子掺杂碳基氧还原(ORR)催化剂具有代替Pt基催化剂的巨大潜力。以硫掺杂g-C3N4(S-doped g-C3N4, S-g-C3N4)作为硫源和氮源,以三嵌段共聚物P123作为碳源,通过简单的高温热解法成功制备了N、S共掺杂碳(N, S co-doped carbon, NSC)催化剂,并考察了热解温度对制备的NSC催化剂ORR性能的影响。材料表征结果显示:温度为1 000 ℃时制备的催化剂NSC-1000具有较高的氮含量和硫含量及最大的比表面积;电化学测试结果显示:NSC-1000具有最佳的ORR性能,在0.1 mol/L KOH溶液中半波电位(half-wave potential, E1/2)高达0.888 V,且经10 000圈循环伏安扫描后E1/2仅负移12 mV,表现出极佳的活性和稳定性。此外,旋转环盘电极测试结果显示:NSC-1000催化剂主要以四电子反应路径催化ORR的发生。本实验为制备N、S共掺杂碳基高效ORR催化剂提供了新的思路。
Abstract:
Heteroatom-doped carbon catalysts have shown great potential to replace Pt-based catalysts for oxygen reduction reaction (ORR). Herein, N, S co-doped carbon (NSC) catalysts were successfully synthesized via a simple high-temperature pyrolysis method with S-doped g-C3N4 (S-g-C3N4) serving as the nitrogen and sulfur sources and triblock copolymer P123 as the carbon source. The effect of pyrolysis temperature on the ORR performance of NSC catalyst was investigated. Characterization shows that the NSC catalyst synthesized at 1 000 ℃ (NSC-1000) has relatively high nitrogen and sulfur content as well as the largest specific surface area. It exhibits the highest ORR activity in alkaline media with a half-wave potential (E1/2) of 0.888 V, and its E1/2 decreases only 12 mV after 10 000 potential cycles, showing excellent catalytic activity and durability. Rotating ring-disk electrode measurement demonstrates the dominant ORR mechanism for NSC-1000 is 4e- transfer. This work provides a novel route for synthesizing highly efficient N, S co-doped carbon catalysts for ORR.

参考文献/References:

[1] ONG W J, TAN L L, NG Y H, et al. Graphitic carbon nitride (g-C3N4)-based photocatalysts for artificial photosynthesis and environmental remediation: are we a step closer to achieving sustainability?[J]. Chemical Reviews, 2016, 116(12): 7159-7329.[2] HAN B, CARLTON C E, KONGKANAND A, et al. Record activity and stability of dealloyed bimetallic catalysts for proton exchange membrane fuel cells [J]. Energy & Environmental Science, 2015, 8(1): 258-266.[3] HUANG W, AHLFIELD J M, KOHL P A, et al. Heat treated tethered iron phthalocyanine carbon nanotube-based catalysts for oxygen reduction reaction in hybrid fuel cells [J]. Electrochimica Acta,2017,257:224-232.[4] JI H Q, WANG M F, LIU S S, et al. Pyridinic and graphitic nitrogen-enriched carbon paper as a highly active bifunctional catalyst for Zn-air batteries [J]. Electrochimica Acta, 2020, 334: 135562.[5] LIAN Y B, YANG W J, ZHANG C F, et al. Unpaired 3D electrons on atomically dispersed cobalt centres in coordination polymers regulate both oxygen reduction reaction (ORR) activity and selectivity for use in zinc-air batteries [J]. Angewandte Chemie, International Edition in English, 2020, 59(1): 286-294.[6] YANG Q, XIAO Z C, KONG D B, et al. New insight to the role of edges and heteroatoms in nanocarbons for oxygen reduction reaction [J]. Nano Energy, 2019, 66: 104096.[7] WANG Z H, JIN H H, MENG T, et al. Fe, Cu-coordinated ZIF-derived carbon framework for efficient oxygen reduction reaction and zinc-air batteries [J]. Advanced Functional Materials, 2018, 28(39): 1802596.[8] SUO N, HUANG H, WU A, et al. Porous boron doped diamonds as metal-free catalysts for the oxygen reduction reaction in alkaline solution [J]. Applied Surface Science, 2018, 439: 329-335.[9] ZHAO Y S, WAN J W, YAO H Y, et al. Few-layer graphdiyne doped with sp-hybridized nitrogen atoms at acetylenic sites for oxygen reduction electrocatalysis [J]. Nature Chemistry, 2018, 10(9): 924-931.[10] ZHANG L, XIONG J, QIN Y H, et al. Porous N-C catalyst synthesized by pyrolyzing g-C3N4 embedded in carbon as highly efficient oxygen reduction electrocatalysts for primary Zn-air battery [J]. Carbon, 2019, 150: 475-484.[11] YU H J, SHANG L, BIAN T, et al. Nitrogen-doped porous carbon nanosheets templated from g-C3N4 as metal-free electrocatalysts for efficient oxygen reduction reaction [J]. Advanced Materials, 2016, 28(25): 5080-5086.[12] HUANG S C, MENG Y Y, CAO Y F, et al. N-, O- and P-doped hollow carbons: metal-free bifunctional electrocatalysts for hydrogen evolution and oxygen reduction reactions [J]. Applied Catalysis B: Environmental, 2019, 248: 239-248.[13] PREUSS K, TǎNASE L C, TEODORESCU C M, et al. Sustainable metal-free carbogels as oxygen reduction electrocatalysts [J]. Journal of Materials Chemistry A, 2017, 5(31): 16336-16343.[14] LI F, DING X B, Cao Q C, et al. A ZIF-derived hierarchically porous Fe-Zn-N-C catalyst synthesized via a two-stage pyrolysis for the highly efficient oxygen reduction reaction in both acidic and alkaline media[J]. Chemical Communications,2019,55(93): 13979-13982.[15] GUO D H, SHIBUYA R, AKIBA C, et al. Active sites of nitrogen-doped carbon materials for oxygen reduction reaction clarified using model catalysts [J]. Science, 2016, 351(6271): 361-365.[16] BEHAN J A, MATES‐TORRES E, STAMATIN S N, et al. Untangling cooperative effects of pyridinic and graphitic nitrogen sites at metal‐free N‐doped carbon electrocatalysts for the oxygen reduction reaction [J]. Small, 2019, 15(48): 1902081.[17] ZHANG L, QIN Y H, YANG L, et al. Multi-role graphitic carbon nitride-derived highly porous iron/nitrogen co-doped carbon nanosheets for highly efficient oxygen reduction catalyst [J]. Journal of Colloid and Interface Science,2021,582:1257-1265.[18] CAO Q C, DING X B, LI F, et al. Zinc, sulfur and nitrogen co-doped carbon from sodium chloride/zinc chloride-assisted pyrolysis of thiourea/sucrose for highly efficient oxygen reduction reaction in both acidic and alkaline media [J]. Journal of Colloid and Interface Science, 2020, 576: 139-146.[19] WANG B W, ZOU J X, SHEN X C, et al. Nanocrystal supracrystal-derived atomically dispersed Mn-Fe catalysts with enhanced oxygen reduction activity [J]. Nano Energy, 2019, 63: 103851[20] LI R R, LIU F, ZHANG Y H, et al. Nitrogen, sulfur co-doped hierarchically porous carbon as a metal-free electrocatalyst for oxygen reduction and carbon dioxide reduction reaction [J]. ACS Applied Materials & Interfaces, 2020,12(40): 44578-44587.[21] ZHANG J Y, ZHANG G, JIN S Y, et al. Graphitic N in nitrogen-doped carbon promotes hydrogen peroxide synthesis from electrocatalytic oxygen reduction [J]. Carbon, 2020, 163: 154-161.[22]  XUE Q, DING Y, XUE Y Y, et al. 3D nitrogen-doped graphene aerogels as efficient electrocatalyst for the oxygen reduction reaction [J]. Carbon, 2018, 139: 137-144.

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备注/Memo

备注/Memo:
收稿日期:2021-05-11基金项目:国家自然科学基金(21306144)作者简介:丁晓波,硕士研究生。E-mail: [email protected]*通讯作者:覃远航,博士,教授。E-mail: [email protected][email protected]引文格式:丁晓波,覃远航. N、S共掺杂碳基高效氧还原催化剂的制备[J]. 武汉工程大学学报,2021,43(4):362-366,390.
更新日期/Last Update: 2021-08-07