氮掺杂诱导Co-Sex活性位点暴露促进MFC中硝酸根催化还原的电子传递途径解析
结题报告
批准号:
21806031
项目类别:
青年科学基金项目
资助金额:
26.0 万元
负责人:
代莹
依托单位:
学科分类:
B0604.水污染与控制化学
结题年份:
2021
批准年份:
2018
项目状态:
已结题
项目参与者:
邹金龙、张敏、梁涛、张鑫、荆宝剑、麻媛媛、陈珲
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中文摘要
硝酸盐氮(NO3--N)是水体富营养化的关键因子之一;高过电位和低效电子利用限制了NO3--N的电催化还原效率。本项目将单室微生物燃料电池(SC-MFC)产电与电催化过程耦合,在以O2为电子受体的SC-MFC中加入NO3--N为共同电子受体;以ZIF-67十二面体为骨架结构、通过钴(Co)中心原位硒化合成的N掺杂诱导表面缺陷(Co−Sex)丰富的二硒化钴/N掺杂石墨化碳(CoSe2/NPGC)为阴极催化剂;考察CoSe2/NPGC结构与活性组分对SC-MFC中NO3--N还原效率、副产物(NO2--N、NH3等)及产电性能的影响;探索与氧还原反应(ORR)共存时,NO3--N在CoSe2/NPGC上还原的活性和稳定性;根据降解有机废水时的产电性能与库伦效率,归纳出NO3--N还原与ORR之间的动态关联,扩展SC-MFC除污染功能,获得NO3--N还原与ORR共存时的电子转移途径与还原机理。
英文摘要
Nitrate (NO3--N) is one of the key factors for water eutrophication. Higher overpotential, inefficient electron availability and utilization limit the electro-catalytic reduction efficiency of NO3--N. In this study, the electricity generation of single-chamber microbial fuel cell (SC-MFC) is coupled with the electro-catalytic process. NO3--N as the shared electron acceptor is added to the SC-MFC with O2 as the initial electron acceptor. Cobalt selenide/N-doped partly-graphitized carbon (CoSe2/NPGC) polyhedron material as the cathode catalyst is prepared from the ZIF-67 dodecahedron and abundant N-induced surface defects (Co-Sex) on CoSe2/NPGC are formed by in-situ selenization of Co. The effects of structure and active components of CoSe2/NPGC on the NO3--N reduction efficiency, the formation of byproducts (NO2--N, NH3, etc) and the electricity generation are investigated. The activity and stability of NO3--N reduction on CoSe2/NPGC cathode is explored in the co-existence of NO3--N and ORR. According to the electricity generation performance and coulombic efficiency during the degradation of organic wastewater in SC-MFC, the dynamic correlations between NO3--N reduction and ORR are studied. Therefore, the decontamination functions of SC-MFC may be expanded and the electron transfer pathway and the reduction mechanism should be obtained when the NO3--N reduction and ORR are simultaneously conducted in SC-MFC.
水体中硝酸盐氮(NO3--N)的存在可能导致严重的环境问题,NO3--N的电催化还原需要一个较高的电势和高效的电子利用率;这就需要一个催化还原NO3--N活性高的催化剂来持续消耗电子,以克服催化过程产生的过电势。(1)通过原位Se化的方法,在不同温度下合成有氧气还原(ORR)或生成反应(OER)活性的CoSe(与NiSe协同)基材料,并通过CoSe/NiSe基催化剂结构的表征、电化学性能优化,使其具有理想的电催化还原活性和稳定性。(2)将MFC过程与电催化还原过程耦合,获得了以Fe3Se4/FeSe基催化剂材料为阴极的MFC降解有机废水的产电性能(1003mW/m2)与库伦效率(25%以上),归纳出ORR与产电性能之间关系的规律性结果,从而扩展MFC的除污染功能,同时发现了电子转移过程为4电子途径。(3)基于ZnO材料具有良好的生物相容性和高OER电位等特点,采用溶剂热-烧结法制备了表面催化活性较高的ZnO/纳米石墨(Nano-G)材料,研究了制备条件对ZnO/Nano-G催化剂结构和性质的影响;并基于电化学性能测试,利用热压法将优选的ZnO/Nano-G材料制备为阴极,对水中NO3--N(100mg/L)的还原效率可以达到82.5%以上,且总氮去除效率在70%以上。
期刊论文列表
专著列表
科研奖励列表
会议论文列表
专利列表
Co3O4@carbon with high Co2þ/Co3þ ratios derived from ZIF-67 supported on N-doped carbon nanospheres as stable bifunctional oxygen catalysts
Co3O4@carbon 具有高 Co2/Co3/3 比率,源自负载在 N 掺杂碳纳米球上的 ZIF-67,作为稳定的双功能氧催化剂
DOI:--
发表时间:2021
期刊:Materials Today Energy
影响因子:9.3
作者:Li Yao;Li Jiahuan;Dai Ying;Li Xuerui;Shao Chunhong;Sun Yubo;Wang Rongyue;Zou Jinlong
通讯作者:Zou Jinlong
Fe3Se4/FeSe heterojunctions in cornstalk-derived N-doped carbon framework enhance charge transfer and cathodic oxygen reduction reaction to boost bio-electricity generation
玉米杆衍生的氮掺杂碳骨架中的 Fe3Se4/FeSe 异质结增强电荷转移和阴极氧还原反应,从而促进生物发电
DOI:10.1016/j.apcatb.2018.11.074
发表时间:2019-05
期刊:Applied Catalysis B: Environmental
影响因子:--
作者:Jing Baojian;You Shijie;Ma Yuanyuan;Xing Zipeng;Chen Hun;Dai Ying;Zhang Chunyue;Ren Nanqi;Zou Jinlong
通讯作者:Zou Jinlong
Self-generated carbon nanotubes for protecting active sites on bifunctional Co/CoOx schottky junctions to promote oxygen reduction/evolution reactions via efficient valence transition
自生成碳纳米管,用于保护双功能 Co/CoOx 肖特基结上的活性位点,通过有效的价态跃迁促进氧还原/放出反应
DOI:10.1016/j.jcis.2019.09.060
发表时间:2019
期刊:Journal of Colloid and Interface Science
影响因子:9.9
作者:Zhang Peng;Cai Zhuang;You Shijie;Wang Fangyu;Dai Ying;Zhang Chunyue;Zhang Yanhong;Ren Nanqi;Zou Jinlong
通讯作者:Zou Jinlong
Carbon-thin-layer protected WP with no passivation supported on acid-treated expanded graphite as efficient Pt Co-catalysts for methanol oxidation and oxygen reduction reactions
碳薄层保护的可湿性粉剂,无钝化,负载在酸处理的膨胀石墨上,作为甲醇氧化和氧还原反应的有效 Pt 助催化剂
DOI:10.1039/c8ta08285e
发表时间:2018-11
期刊:Journal of Materials Chemistry A
影响因子:11.9
作者:Zhang Chunyue;Dai Ying;Chen Hun;Ma Yuanyuan;Jing Baojian;Cai Zhuang;Duan Yaqiang;Tang Bo;Zou Jinlong
通讯作者:Zou Jinlong
ZIF-8-derived carbon-thin-layer protected WC/W24O68 micro-sized rods with enriched oxygen vacancies as efficient Pt co-catalysts for methanol oxidation and oxygen reduction
ZIF-8衍生的具有富氧空位的碳薄层保护WC/W24O68微米棒作为甲醇氧化和氧还原的高效Pt助催化剂
DOI:10.1016/j.apcatb.2019.118574
发表时间:2020-05
期刊:Applied Catalysis B: Environmental
影响因子:--
作者:Li Jiahuan;You Shijie;Liu Mingyang;Zhang Peng;Dai Ying;Yu Yang;Ren Nanqi;Zou Jinlong
通讯作者:Zou Jinlong
国内基金
海外基金