g-C_3N_4/双钙钛矿复合材料的制备及氧催化性能
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摘要
通过溶胶-凝胶法制备出不同Ni掺杂比例的双钙钛矿Sr_2Ni_xCo_(2-x)O_6(x=0.2,0.4,0.6,0.8),通过热分解法制备出具有层状结构的纳米颗粒g-C_3N_4,并制备其复合物催化剂。将双钙钛矿和g-C_3N_4分别制备成双功能电极片,用于测试其对氧还原(ORR)和氧析出(OER)的催化活性,然后选取具有最佳氧催化活性的Ni掺杂比例x=0.4的双钙钛矿与一定重量比例的g-C_3N_4进行复合,测试复合催化剂的氧催化活性。结果表明,复合后的催化剂催化效果明显优于单一催化剂,当g-C_3N_4添加量占双钙钛矿的30%(w/w)时复合催化剂催化氧还原反应的最大电流密度为395.7 mA·cm~(-2)(-0.6 V vs Hg/HgO),氧析出反应的最大电流密度为372.0mA·cm~(-2)(1 V vs Hg/HgO),这表明g-C_3N_4与Sr_2Ni_(0.4)Co_(1.6)O_6复合后协同催化能够提高双钙钛矿的氧催化活性。
Double perovskite Sr_2Ni_xCo_(2-x)O_6(x=0.2,0.4,0.6,0.8)with different Ni doping ratios were prepared by sol-gel method,and nanoparticles g-C_3N_4with layered structure was prepared by thermal decomposition.Synthesis of double perovskite and g-C_3N_4composite that were used as bifunctional catalysts,which were prepared into bifunctional electrodes,and used to test its catalytic activity for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).Then,the doping ratio(x=0.4)of Ni in double perovskite with the best oxygen catalytic activity was selected to be composited with a certain weight ratio of g-C_3N_4,testing the catalytic activity of the composite catalysts.The results show that the composite catalysts were obviously better than the single catalysts.When the amount of g-C_3N_4added was 30%of the mass of the double perovskite,the maximum current densities of the catalytic ORR was 395.7 mA·cm~(-2)(-0.6 V vs Hg/HgO),the catalytic OER was 372.0 mA·cm~(-2)(1 V vs Hg/Hg O).This indicates that the synergistic catalysis of g-C_3N_4and Sr_2Ni_(0.4)Co_(1.6)O_6could improve the catalytic activity of the double perovskite.
Double perovskite Sr_2Ni_xCo_(2-x)O_6(x=0.2,0.4,0.6,0.8)with different Ni doping ratios were prepared by sol-gel method,and nanoparticles g-C_3N_4with layered structure was prepared by thermal decomposition.Synthesis of double perovskite and g-C_3N_4composite that were used as bifunctional catalysts,which were prepared into bifunctional electrodes,and used to test its catalytic activity for oxygen reduction reaction(ORR)and oxygen evolution reaction(OER).Then,the doping ratio(x=0.4)of Ni in double perovskite with the best oxygen catalytic activity was selected to be composited with a certain weight ratio of g-C_3N_4,testing the catalytic activity of the composite catalysts.The results show that the composite catalysts were obviously better than the single catalysts.When the amount of g-C_3N_4added was 30%of the mass of the double perovskite,the maximum current densities of the catalytic ORR was 395.7 mA·cm~(-2)(-0.6 V vs Hg/HgO),the catalytic OER was 372.0 mA·cm~(-2)(1 V vs Hg/Hg O).This indicates that the synergistic catalysis of g-C_3N_4and Sr_2Ni_(0.4)Co_(1.6)O_6could improve the catalytic activity of the double perovskite.
引文
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[6] WANG Ying(王瀛), ZHANG Li-Min(张丽敏), HU Tian-Jun(胡天军). Acta Chim. Sinica(化学学报), 2015,73(4):316-325
[7] You S J, Gong X B, Wang W, et al. Adv. Energy Mater.,2016,6(1):1501497
[8] Huang Q S, Zhou P J, Yang H, et al. Electrochim. Acta,2017,232:339-347
[9] Li X, Wang H J, Yu H, et al. J. Power Sources, 2014,260:1-5
[10]Singh P, Buttry D A. J. Phys. Chem. C, 2012,116(19):10656-10663
[11]Alia S M, Zhang G, Kisailus D, et al. Adv. Funct. Mater.,2010,20(21):3742-3746
[12]ZHUANG Shu-Xin(庄树新), L譈Jian-Xian(吕建先), LU Mi(路密), et al. Prog. Chem.(化学进展), 2015,27(4):436-447
[13]Bie S Y, Zhu Y Q, Su J M, et al. J. Mater. Chem. A, 2015,3(44):22448-22453
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[15]Falcón H, Barbero J A, Araujo G, et al. Appl. Catal. B,2004,53(1):37-45
[16]Brieuc F, Dezanneau G, Hayoun M, et al. Solid State Ionics,2017,309:187-191
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[18]YU Wen-Wan(于文婉), HUANG Hong-Xia(黄红霞), WANG Cheng(王成). Chinese J. Inorg. Chem.(无机化学学报),2018,34(3):475-482
[19]Sun N, Liu H X, Yu Z Y, et al. Ionics, 2016,22:869-876
[20]Zhao K, Li L W, Zheng A Q, et al. Appl. Energy, 2017,197:393-404
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[22]Chen X F, Zhang J S, Fu X Z, et al. J. Am. Chem. Soc.,2009,131(33):11658-11659
[23]Wu Y X, Wang T H, Zhang Y D, et al. Sci. Rep., 2016,6:24314
[24]Liao G Z, Chen S, Quan X, et al. J. Mater. Chem., 2012,22(6):2721-2726
[25]WU Yan-Bo(吴艳波), BI Jun(毕军), WEI Bin-Bin(魏斌斌).Acta Phys.-Chim. Sin.(物理化学学报), 2015,31:315-321
[26]Holzwarth U, Gibson N. Nat. Nanotechnol., 2011,6(9):534
[27]Yin X, Hong L. Appl. Catal. A, 2009,371(1):153-160
[28]Dang X M, Zhang X F, Chen Y T, et al. J. Nanopart. Res.,2015,17(2):93
[29]Fabbri E, Mohamed R, Levecque P, et al. ChemElectroChem,2014,1(2):338-342
[30]Wu Z L, Sun L P, Xia T, et al. J. Power Sources, 2016,334:86-93
[31]Cheriti M, Kahoul A. Mater. Res. Bull., 2012,47(1):135-141