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基于第一性原理的密度泛函理论研究了B, P单掺杂以及B, P共掺杂石墨烯对O, O2, OH和OOH的吸附特性. 通过分析吸附能、键长、 态密度以及电荷转移, 比较了不同掺杂对燃料电池氧还原反应(ORR)中间物吸附的影响, 进而探讨了反应过程, 并给出各步反应自由能的变化趋势. 结果表明: B, P单掺杂石墨烯对各中间物的吸附能存在线性关系, 掺P石墨烯吸附OOH的吸附能为3.26 eV, 远大于掺B石墨烯的吸附能0.73 eV; 掺P石墨烯较大的吸附能有利于中间物OOH中OO键的断裂, 掺B石墨烯吸附能小有利于中间物OH生成H2O脱附的反应发生; 而B, P 共掺杂石墨烯的吸附存在协同效应, 具有更好的催化ORR的反应能力.
[1] Shao A F, Wang Z B, Chu Y Y, Jiang Z Z, Yin G P, Liu Y 2010 Fuel Cells 10 472
[2] Nagashree K L, Raviraj N H, Ahmed M F 2010 Electrochim. Acta 55 2629
[3] Gasteiger H A, Markovic N M 2009 Science 324 48
[4] Gong K P, Du F, Xia Z H, Durstock M, Dai L M 2009 Science 323 760
[5] Liu X, Li L, Meng C G, Han Y 2012 J. Phys. Chem. C 116 2710
[6] Neergat M, Shukla A K, Gandhi K S 2001 J. Appl. Electrochem. 31 373
[7] Yu X W, Ye S Y 2007 J. Power Sources 172 145
[8] Novoselov K S, Geim A K, Morozov S V, Jiang D, Zhang Y, Dubonos S V, Grigorieva I V, Firsov A A 2004 Science 306 666
[9] Novoselov K S, Geim A K, Morozov S V, Jiang D, Katsnelson M I, Grigorieva I V, Dubonos S V, Firsov A A 2005 Nature 438 197
[10] Lee C G, Wei X D, Kysar J W, Home J 2008 Science 321 385
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[18] Ma G X, Zhao J H, Zheng J F, Zhu Z P 2012 New Carbon Mater. 27 258
[19] Yang Z, Yao Z, Li G F, Fang G Y, Nie H G, Liu Z, Zhou X M, Chen X A, Huang S M 2012 ACS Nano 6 205
[20] Tang L H, Wang Y, Li Y M, Feng H B, Lu J, Li J H 2009 Adv. Funct. Mater. 19 2782
[21] Sun X J, Zhang Y W, Song P, Pan J, Zhuang L, Xu W L, Xing W 2013 ACS Catal. 3 1726
[22] Yao Z, Nie H G, Yang Z, Zhou X M, Liu Z, Huang S M 2012 Chem. Commun. 48 1027
[23] Sheng Z H, Gao H L, Bao W J, Wang F B, Xia X H 2012 J. Mater. Chem. 22 390
[24] Chen Y H, Tian Y Y, Fang X Z, Liu J G, Yan C W 2014 Electrochim. Acta 143 291
[25] Li R, Wei Z D, Gou X L, Xu W 2013 RSC Adv. 3 9978
[26] Zhang C Z, Mahmood N, Yin H, Liu F, Hou Y L 2013 Adv. Mater. 25 4932
[27] Ozaki J I, Kimura N, Anahara T, Oya A 2007 Carbon 45 1847
[28] Zhu J L, He C Y, Li Y Y, Kang S A, Shen P K 2013 J. Mater. Chem. A 1 14700
[29] Zheng Y, Jiao Y, Ge L, Jaroniec M, Qiao S Z 2013 Angew. Chem. Int. Ed. 52 3110
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[31] Duan X G, Indrawirawan S, Sun H Q, Wang S B 2015 Catal. Today 249 184
[32] Kong X K, Chen Q W, Sun Z Y 2013 Chem. Phys. Chem. 14 514
[33] Zhang X L, Lu Z S, Fu Z M, Tang Y N, Ma D W, Yang Z X 2015 J. Power Sources 276 222
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[39] Zhang H Q, Liang Y M, Zhou J X 2014 Acta Chim. Sin. 72 367
-
[1] Shao A F, Wang Z B, Chu Y Y, Jiang Z Z, Yin G P, Liu Y 2010 Fuel Cells 10 472
[2] Nagashree K L, Raviraj N H, Ahmed M F 2010 Electrochim. Acta 55 2629
[3] Gasteiger H A, Markovic N M 2009 Science 324 48
[4] Gong K P, Du F, Xia Z H, Durstock M, Dai L M 2009 Science 323 760
[5] Liu X, Li L, Meng C G, Han Y 2012 J. Phys. Chem. C 116 2710
[6] Neergat M, Shukla A K, Gandhi K S 2001 J. Appl. Electrochem. 31 373
[7] Yu X W, Ye S Y 2007 J. Power Sources 172 145
[8] Novoselov K S, Geim A K, Morozov S V, Jiang D, Zhang Y, Dubonos S V, Grigorieva I V, Firsov A A 2004 Science 306 666
[9] Novoselov K S, Geim A K, Morozov S V, Jiang D, Katsnelson M I, Grigorieva I V, Dubonos S V, Firsov A A 2005 Nature 438 197
[10] Lee C G, Wei X D, Kysar J W, Home J 2008 Science 321 385
[11] Sun J P, Miao Y M, Cao X C 2013 Acta Phys. Sin. 62 036301 (in Chinese) [孙建平, 缪应蒙, 曹相春 2013 物理学报 62 036301]
[12] Huang L Q, Zhou L Y, Yu W, Yang D, Zhang J, Li C 2015 Acta Phys. Sin. 64 038103 (in Chinese) [黄林泉, 周玲玉, 于为, 杨栋, 张坚, 李灿 2015 物理学报 64 038103]
[13] Yang X X, Kong X T, Dai Q 2015 Acta Phys. Sin. 64 106801 (in Chinese) [杨晓霞, 孔祥天, 戴庆 2015 物理学报 64 106801]
[14] Zhao J, Zhang G Y, Shi D X 2013 Chin. Phys. B 22 057701
[15] Wu H Q, Linghu C Y, L H M, Qian H 2013 Chin. Phys. B 22 098106
[16] Yang L J, Jiang S J, Zhao Y, Zhu L, Chen S, Wang X Z, Wu Q, Ma J, Ma Y W, Hu Z 2011 Angew. Chem. Int. Ed. 50 7132
[17] Qu L T, Liu Y, Baek J B, Dai L M 2010 ACS Nano 4 1321
[18] Ma G X, Zhao J H, Zheng J F, Zhu Z P 2012 New Carbon Mater. 27 258
[19] Yang Z, Yao Z, Li G F, Fang G Y, Nie H G, Liu Z, Zhou X M, Chen X A, Huang S M 2012 ACS Nano 6 205
[20] Tang L H, Wang Y, Li Y M, Feng H B, Lu J, Li J H 2009 Adv. Funct. Mater. 19 2782
[21] Sun X J, Zhang Y W, Song P, Pan J, Zhuang L, Xu W L, Xing W 2013 ACS Catal. 3 1726
[22] Yao Z, Nie H G, Yang Z, Zhou X M, Liu Z, Huang S M 2012 Chem. Commun. 48 1027
[23] Sheng Z H, Gao H L, Bao W J, Wang F B, Xia X H 2012 J. Mater. Chem. 22 390
[24] Chen Y H, Tian Y Y, Fang X Z, Liu J G, Yan C W 2014 Electrochim. Acta 143 291
[25] Li R, Wei Z D, Gou X L, Xu W 2013 RSC Adv. 3 9978
[26] Zhang C Z, Mahmood N, Yin H, Liu F, Hou Y L 2013 Adv. Mater. 25 4932
[27] Ozaki J I, Kimura N, Anahara T, Oya A 2007 Carbon 45 1847
[28] Zhu J L, He C Y, Li Y Y, Kang S A, Shen P K 2013 J. Mater. Chem. A 1 14700
[29] Zheng Y, Jiao Y, Ge L, Jaroniec M, Qiao S Z 2013 Angew. Chem. Int. Ed. 52 3110
[30] Choi C H, Park S H, Woo S I 2012 J. Mater. Chem. 22 12107
[31] Duan X G, Indrawirawan S, Sun H Q, Wang S B 2015 Catal. Today 249 184
[32] Kong X K, Chen Q W, Sun Z Y 2013 Chem. Phys. Chem. 14 514
[33] Zhang X L, Lu Z S, Fu Z M, Tang Y N, Ma D W, Yang Z X 2015 J. Power Sources 276 222
[34] Fan X F, Zheng W T, Kuo J L 2013 RSC Adv. 3 5498
[35] Norskov J K, Rossmeisl J, Logadottir A, Lindqvist L 2004 J. Phys. Chem. B 108 17886
[36] Li M T, Zhang L P, Xu Q, Niu J B, Xia Z H 2014 J. Catal. 314 66
[37] Lim D H, Wilcox J 2012 J. Phys. Chem. C 116 3653
[38] Atkins P W 1998 Physical Chemistry (6th Ed.) (Oxford: Oxford University Press) pp485, 925-927, 942
[39] Zhang H Q, Liang Y M, Zhou J X 2014 Acta Chim. Sin. 72 367
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