ZIF-67衍生的Ag/Co@NC材料及其氧还原性能的研究

doi:10.13208/j.electrochem.180726

电化学（中英文） ›› 2019, Vol. 25 ›› Issue (6): 781-791. doi: 10.13208/j.electrochem.180726

ZIF-67衍生的Ag/Co@NC材料及其氧还原性能的研究

狄正玲^1,2，朱靖^1,2，戴磊^1,2*，孟伟^1,2，李跃华^1,2，何章兴^1,2，王岭^1,2

1. 华北理工大学化学工程学院，河北唐山 063210； 2. 河北省环境光电催化材料重点实验室，河北唐山 063009

收稿日期:2018-07-27 修回日期:2018-08-28 出版日期:2019-12-28 发布日期:2019-12-28
通讯作者: 戴磊 E-mail:dailei_b@163.com
基金资助:
国家自然科学基金(No. 51772097)，河北省杰出青年基金(No. E2017209079)，河北省自然科学基金(No. B2016109266)

ZIF-67-Derived Ag/Co-Embedded N-Enriched Mesoporous Carbon for Oxygen Reduction Reaction

DI Zheng-ling^1,2, ZHU Jing^1,2, DAI Lei^1,2*, MENG Wei^1,2, LI Yue-hua^1,2,HE Zhang-xing^1,2, WANG Ling^1,2

1. College of Chemical Engineering, North China University of Science and Technology, Tangshan 063210, PR China; 2. Hebei Province Key Laboratory of Photocatalytic and Electrocatalytic Materials for Environment, Tangshan 063009, PR China

Received:2018-07-27 Revised:2018-08-28 Published:2019-12-28 Online:2019-12-28
Contact: DAI Lei E-mail:dailei_b@163.com
Supported by:
The project was supported by the Natural Science Foundation of China (No. 51772097), Hebei Natural Science Funds for Distinguished Young Scholar (No. E2017209079) and Hebei Natural Science Fund (No. B2016209266).

摘要/Abstract

摘要： 氮掺杂的多孔碳材料可作为氧还原反应的催化剂，本文借助ZIF-67富氮多孔的特殊结构，采用湿式逐步还原法将Ag嵌入ZIF-67孔腔内，然后在Ar中碳化成功地制备了Ag/Co双金属嵌入的氮掺杂的多孔碳复合材料（Ag/Co@NC）作为氧还原反应的催化剂. 为了证明Ag的突出作用，同时在Ar中碳化了ZIF-67制备了Co嵌入的氮掺杂的多孔碳材料（Co@NC）. 利用扫描电子显微镜、透射电子显微镜、X射线衍射、X射线光电子能谱以及比表面积分析对材料的显微形貌、物相组成、结构进行分析，采用循环伏安和线性扫描极化曲线对材料的氧还原催化活性和催化稳定性进行研究. 结果表明，Ag的嵌入未改变ZIF-67的晶体结构，但是大大提高了材料的氧还原催化活性. Ag/Co@NC材料的半波电位和起始电位均高于Co@NC材料，且其在1000次循环伏安测试前后的半波电位变化仅为30 mV，显示出很好的催化稳定性和甲醇耐受性，可作为燃料电池和金属-空气电池的阴极催化剂.

关键词: 氧还原, ZIF-67, 氮掺杂的多孔碳, 银纳米粒子

Abstract: Nitrogen-doped porous carbon materials are considered as one of the most promising catalysts for oxygen reduction reaction (ORR). Herein, in order to further improve the activity of the nitrogen-doped porous carbon, Ag/Co bimetal is embedded into nitrogendoped porous carbon to form Ag/Co-embedded nitrogen-doped porous carbon material (AgCo@NC). The AgCo@NC was derived by the wet impregnation of Ag+ into ZIF-67 precursor, followed by chemical reduction and a subsequent pyrolysis process under Ar atmosphere at different temperatures (500 ℃, 600 ℃, 700 ℃). The morphologic characterization shows that the Ag/Co nanoparticles were successfully embedded in the mesoporous carbon framework with abundant nitrogen atoms. The electrochemical test results indicate that the AgCo@NC-600 catalyst exhibited the higher onset potential and half-wave potential than thods of others and Pt/C in alkaline media. Furthermore, the AgCo@NC and Co@NC also displayed the higher methanol-tolerance performance than commercial Pt/C.

Key words: oxygen reduction reaction, ZIF-67, N-doped porous carbon, Ag nanoparticles

中图分类号:

Q81
O646.54

狄正玲, 朱靖, 戴磊, 孟伟, 李跃华, 何章兴, 王岭. ZIF-67衍生的Ag/Co@NC材料及其氧还原性能的研究[J]. 电化学（中英文）, 2019, 25(6): 781-791.

DI Zheng-ling, ZHU Jing, DAI Lei, MENG Wei, LI Yue-hua, HE Zhang-xing, WANG Ling. ZIF-67-Derived Ag/Co-Embedded N-Enriched Mesoporous Carbon for Oxygen Reduction Reaction[J]. Journal of Electrochemistry, 2019, 25(6): 781-791.

导出引用管理器 EndNote|Ris|BibTeX

链接本文: https://electrochem.xmu.edu.cn/CN/10.13208/j.electrochem.180726

https://electrochem.xmu.edu.cn/CN/Y2019/V25/I6/781

参考文献

[1] Zhang Z W, Li H N, Hu J, et al. High oxygen reduction reaction activity of C-N/Ag hybrid composites for Zn-air battery[J]. Journal of Alloys And Compounds, 2016, 694: 419-428.
[2] Men B, Sun Y Z, Tang Y, et al. Highly dispersed Ag-functionalized graphene electrocatalyst for oxygen reduction reaction in energy-saving electrolysis of sodium carbonate[J]. Industrial & Engineering Chemistry Research, 2015, 54(30): 7415-7422.
[3] Wang Y, Lu X J, Liu Y, et al. Silver supported on Co₃O₄, modified carbon as electrocatalyst for oxygen reduction reaction in alkaline media[J]. Electrochemistry Communications, 2013, 31: 108-111.
[4] Wang Y, Liu Y, Lu X J, et al. Silver-molybdate electrocatalysts for oxygen reduction reaction in alkaline media[J]. Electrochemistry Communications, 2012, 20: 171-174.
[5] Wang Y, Liu Q, Zhang L M, et al. One-pot synthesis of Ag-CoFe₂O₄/C as efficient catalyst for oxygen reduction in alkaline media[J]. International Journal of Hydrogen Energy, 2016, 41(47): 22547-22553.
[6] Meng H, Shen P K. Novel Pt-free catalyst for oxygen electroreduction[J]. Electrochemistry Communications[J]. 2006, 8(4): 588-594.
[7] Soo L T, Loh K S, Mohamad A, et al. Synthesis of silver/nitrogen-doped reduced graphene oxide through a one-step thermal solid-state reaction for oxygen reduction in an alkaline medium[J]. Journal of Power Sources, 2016, 324: 412-420.
[8] Ruiz-Camacho B, Martínez Álvarez O, Rodríguez-Santoyo H H, et al. Mono and bi-metallic electrocatalysts of Pt and Ag for oxygen reduction reaction synthesized by sonication[J]. Electrochemistry Communications, 2015, 61: 5-9.
[9] Cheng Y H, Li W Y, Fan X Z, et al. Modified multi-walled carbon nanotube/Ag nanoparticle composite catalyst for the oxygen reduction reaction in alkaline solution[J]. Electrochimica Acta, 2013, 111: 635-641.
[10] Wang Y C, Wu H B, Jiang X E. Facile-green synthesis of nitrogen-doped carbon-supported ultrafine silver catalyst with enhanced electrocatalytic property[J]. Electrochimica Acta, 2013, 108(10): 66-73.
[11] Jiang T T, Wang Y, Wang K, et al. A novel sulfur-nitrogen dual doped ordered mesoporous carbon electrocatalyst for efficient oxygen reduction reaction[J]. Applied Catalysis B - Environmental, 2016, 189: 1-11.
[12] Yu H Y, Fisher A , Cheng D J, et al. Cu, N-codoped hierarchical porous carbons as electrocatalysts for oxygen reduction reaction[J]. ACS Applied Materials & Interfaces, 2016, 8(33): 21431-21439.
[13] Tan C, Wang F, Liu J J, et al. An easy route to prepare carbon black-silver hybrid catalysts for electro-catalytic oxidation of hydrazine[J]. Materials Letters, 2009, 63(12): 969-971.
[14] Xu X H, Tan C, Liu H J, et al. Carbon black supported ultra-high loading silver nanoparticle catalyst and its enhanced electrocatalytic activity towards oxygen reduction reaction in alkaline medium[J]. Journal of Electroanalytical Chemistry, 2013, 696(8): 9-14.
[15] Niu Q J, Guo J X, Chen B L, et al. Bimetal-organic frameworks/polymer core-shell nanofibers derived heteroatom-doped carbon materials as electrocatalysts for oxygen reduction reaction[J]. Carbon, 2016, 114: 250-260.
[16] Lu H S, Zhang H M, Liu R R, et al. Macroscale cobalt-MOFs derived metallic Co nanoparticles embedded in N-doped porous carbon layers as efficient oxygen electrocatalysts[J]. Applied Surface Science, 2017, 392: 402-409.
[17] Long J L, Li R, Gou X L. Well-organized Co-Ni@NC material derived from hetero-dinuclear MOFs as efficient electrocatalysts for oxygen reduction[J]. Catalysis Communications, 2017, 95: 31-35.
[18] Jiang M, He H, Yi W J, et al. ZIF-67 derived Ag-Co₃O₄ @N-doped carbon/carbon nanotubes composite and its application in Mg-air fuel cell[J]. Electrochemistry Communications, 2017, 77: 5-9.
[19] Qian Y H, Hu Z G, Ge X M, et al. A metal-free ORR/OER bi-functional electrocatalyst derived from metal-organic frameworks for rechargeable Zn-Air batteries[J]. Carbon, 2016, 111: 641-650.
[20] Ying J, Li J, Jiang G P, et al. Metal-organic frameworks derived platinum-cobalt bimetallic nanoparticles in nitrogen-doped hollow porous carbon capsules as a highly active and durable catalyst for oxygen reduction reaction[J]. Applied Catalysis B - Environmental, 2018, 225: 496-503
[21] Thomas M, Illathvalappi R, Kurungot S, et al. Graphene oxide sheathed ZIF-8 microcrystals: engineered precursors of nitrogen-doped porous carbon for efficient oxygen reduction reaction (ORR) electrocatalysis[J]. ACS Applied Materials & Interfaces, 2016, 8(43): 29373-29382.
[22] Ahn S H, Manthiram A. Self-templated synthesis of Co- and N-doped carbon microtubes composed of hollow nanospheres and nanotubes for efficient oxygen reduction reaction[J]. Small, 2017, 13(11): 160343.
[23] He L, Weniger F, Neumann H, et al. Synthesis, characterization, and application of metal nanoparticles supported on nitrogen-doped carbon: catalysis beyond electrochemistry[J]. Angewandte Chemie International Edition, 2016, 47(48): 12582-12594.
[24] Zhou X J, Bai Z Y, Wu M J, et al. 3-dimensional porous N-doped graphene foam as a non-precious catalyst for the oxygen reduction reaction[J] Journal of Materials Chemistry A, 2015, 3(7): 3343-3350.
[25] Lai C L, Kolla P, Zhao Y, et al. Lignin-derived electrospun carbon nanofiber mats with supercritically deposited Ag nanoparticles for oxygen reduction reaction in alkaline fuel cells[J]. Electrochimica Acta, 2014, 130: 431-438.
[26] Cao J Y, Guo M W, Wu J Y, et al. Carbon-supported Ag@Pt core-shell nanoparticles with enhanced electrochemical activity for methanol oxidation and oxygen reduction reaction[J]. Journal of Power Sources, 2015, 277: 155-160.
[27] Cheng Y H, Tian Y Y, Tsang S W, et al. Ag nanoparticles on boron doped multi-walled carbon nanotubes as a synergistic catalysts for oxygen reduction reaction in alkaline media[J]. Electrochimica Acta, 2015, 174: 919-924.
[28] Yasuda S, Furuya A, Uchibori Y, et al. Iron-nitrogen-doped vertically aligned carbon nanotube electrocatalyst for the oxygen reduction reaction[J]. Advanced Functional Materials, 2016, 26(5): 738-744.
[29] Ju J(鞠剑), Chen W(陈卫). Synthesis of silver nanoparticles supported on graphene quantum dots for oxygen reduction reaction[J]. Journal of Electrochemistry(电化学), 2014, 20(4): 353-359.
[30] Xia W, Mahmood A, Liang Z B, et al. Earth-abundant nanomaterials for oxygen reduction[J]. Angewandte Chemie International Edition, 2016, 55(8): 2650-2676.
[31] Jiang M X(姜梦秀), Zhang J(张晶), Li Y H(李月华), et al. Cobalt-based nitrogen-doped carbon non-noble metal catalysts for oxygen reduction reaction[J]. Journal of Electrochemistry(电化学), 2017, 23(6): 627-637.
[32] Ai K L, Li Z L, Cui X Q. Scalable preparation of sized-controlled Co-N-C electrocatalyst for efficient oxygen reduction reaction[J]. Journal of Power Sources, 2017, 368: 46-56.
[33] Zhang H Y, Tian Y, Zhao J X, et al. Small dopants make big differences: enhanced electrocatalytic performance of MoS₂, monolayer for oxygen reduction reaction (ORR) by N- and P-doping[J]. Electrochimica Acta, 2017, 225: 543-550.
[34] Wang H H, Wang C N, Liu L, et al. Synthesis of Co-Fe-Pd nanoparticles via ultrasonic irradiation and their electro-catalytic activity for oxygen reduction reaction[J]. Applied Catalysis A - General, 2018, 560: 103-110.
[35] Lu H S, Zhang H , Zhang X, et al. Transformation of carbon-encapsulated metallic Co into ultrafine Co/CoO nanoparticles exposed on N-doped graphitic carbon for high-performance rechargeable zinc-air battery[J]. Applied Surface Science, 2018, 448: 369-379.
[36] Pels J R, Kapteijn F, Moulijn J A, et al. Evolution of nitrogen functionalities in carbonaceous materials during pyrolysis[J]. Carbon, 1995, 33(11): 1641-1653.
[37] Huang X Q, Zhao Z P, Cao L, et al. High-performance transition metal-doped Pt₃Ni octahedra for oxygen reduction reaction[J]. Science, 2015, 348(6240): 1230-1234.

ZIF-67衍生的Ag/Co@NC材料及其氧还原性能的研究

ZIF-67-Derived Ag/Co-Embedded N-Enriched Mesoporous Carbon for Oxygen Reduction Reaction

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

Metrics

[1]	陈发东, 谢卓洋, 李孟婷, 陈四国, 丁炜, 李莉, 李静, 魏子栋. 系列综述（1/4）:重庆大学魏子栋教授课题组在电化学能源转换方面的研究进展：燃料电池高性能氧还原催化剂[J]. 电化学（中英文）, 2024, 30(7): 2314007-.
[2]	郑天龙, 欧明玉, 徐松, 毛信表, 王释一, 和庆钢. 一体式可再生燃料电池双功能氧催化剂的研究进展[J]. 电化学（中英文）, 2023, 29(7): 2205301-.
[3]	刘思淼, 周景娇, 季世军, 文钟晟. FeNi-CoP/NC双功能催化剂的制备及电催化性能研究[J]. 电化学（中英文）, 2023, 29(10): 211118-.
[4]	王健, 轩文辉, 何倩, 蒋金霞, 周圆圆, 聂瑶, 廖强, 邵敏华, 丁炜, 魏子栋. 类超晶格结构：有序性传质赋予燃料电池高品质输出性能[J]. 电化学（中英文）, 2023, 29(1): 2215003-.
[5]	郭鸿波, 王亚妮, 郭凯, 雷海涛, 梁作中, 张学鹏, 曹睿. 吸电子和亲水性Co-卟啉促进电催化氧还原反应的研究[J]. 电化学（中英文）, 2022, 28(9): 2214002-.
[6]	张天恩, 颜雅妮, 张俊明, 瞿希铭, 黎燕荣, 姜艳霞. 调控Pt₃Zn合金化程度改善酸性氧还原活性与稳定性[J]. 电化学（中英文）, 2022, 28(4): 2106091-.
[7]	冯雅辰, 王翔, 王宇琪, 严会娟, 王栋. 电催化氧还原反应的原位表征[J]. 电化学（中英文）, 2022, 28(3): 2108531-.
[8]	袁会芳, 张越, 翟兴吾, 胡立兵, 葛桂贤, 王刚, 于锋, 代斌. 氮掺杂碳原位锚定铜纳米颗粒用于高效氧还原反应催化剂[J]. 电化学（中英文）, 2021, 27(6): 671-680.
[9]	林华, 吴艺津, 李君涛, 周尧. 一锅法制备Fe₂O₃@Fe-N-C氧还原电催化剂及其锌-空气电池的性能研究[J]. 电化学（中英文）, 2021, 27(4): 366-376.
[10]	李文杰, 田东旭, 杜红, 燕希强. ORR催化剂Ni_m@Pt₁Au_n_-_m_-1(n = 19, 38, 55, 79; m = 1, 6, 13, 19)的密度泛函研究[J]. 电化学（中英文）, 2021, 27(4): 357-365.
[11]	刘芳艳, 张倩, 李玥琨, 黄丰, 王梦晔. Co_1-_xS-MnS@CNTs/CNFs的制备及其氧还原电催化性能[J]. 电化学（中英文）, 2021, 27(3): 301-310.
[12]	吴志鹏, 钟传建. 钯基氧还原和乙醇氧化反应电催化剂:关于结构和机理研究的一些近期见解[J]. 电化学（中英文）, 2021, 27(2): 144-156.
[13]	徐明俊, 刘杰, 葛君杰, 刘长鹏, 邢巍. 长春应化所金属氮碳氧还原催化剂的研究进展[J]. 电化学（中英文）, 2020, 26(4): 464-473.
[14]	徐能能, 乔锦丽. 锌-空气电池双功能催化剂研究进展[J]. 电化学（中英文）, 2020, 26(4): 531-562.
[15]	姚硕, 黄太仲, RizwanHaider, 房恒义, 于洁玫, 姜占坤, 梁栋, 孙玥, 原鲜霞. NiO@rGO负载钯、银纳米粒子用作氧还原催化剂[J]. 电化学（中英文）, 2020, 26(2): 270-280.