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电化学析氢反应中单层MoSe2氢吸附机理第一性原理研究

徐紫巍 石常帅 赵光辉 王明渊 刘桂武 乔冠军

电化学析氢反应中单层MoSe2氢吸附机理第一性原理研究

徐紫巍, 石常帅, 赵光辉, 王明渊, 刘桂武, 乔冠军
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  • 基于密度泛函理论的第一性原理方法,本文计算了单层2H相MoSe2纳米材料表面及两种边缘(Mo原子边缘、Se原子边缘)不同活性位点、不同氢原子吸附率下的氢吸附吉布斯自由能(Gibbs free energy,用△GH0表示),并且将对应的微观结构进行了系统分析比较,得出△GH0最接近于0 eV的吸附位点及相应的吸附率.同时,结合差分电荷密度和电负性理论,分析了单层MoSe2两种边缘氢吸附的电荷转移及成键特性,进一步解释了不同吸附位点呈现的结构与能量趋势.最后,通过基于密度泛函理论的第一性原理分子动力学模拟,研究了高温热运动对两种边缘氢吸附的影响,获得了氢原子发生脱附的临界温度及对应的微观动态过程.该理论研究从原子尺度揭示了单层2H相MoSe2纳米材料边缘不同位点在不同温度下对氢原子吸附和脱附的微观机理,证实了Mo原子边缘的畸变和重构行为,加深了对实验中单层2H相MoSe2边缘在不同温度下氢吸附机理的理解,为实验中通过控制MoSe2边缘设计廉价高效的析氢催化剂提供理论参考.
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    [2]

    Radisavljevic B, Radenovic A, Brivio J, Giacometti I V, Kis A 2011 Nat. Nanotechnol. 6 147

    [3]

    Chhowalla M, Shin H S, Eda G, Li L J, Loh K P, Zhang H 2013 Nat. Chem. 5 263

    [4]

    Frame F A, Osterloh F E 2010 J. Phys. Chem. C 114 10628

    [5]

    Huang M, Cho K 2009 J. Phys. Chem. C 113 5238

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    Liu Z K, Lau S P, Yan F 2015 Chem. Soc. Rev. 44 5638

    [7]

    Xiang Q J, Yu J G, Jaroniec M 2012 J. Am. Chem. Soc. 134 6575

    [8]

    Ding Q, Meng F, English C R, Caban-Acevedo M, Shearer M J, Liang D, Daniel A S, Hamers R J, Jin S 2014 J. Am. Chem. Soc. 136 8504

    [9]

    Chang K, Mei Z W, Wang T, Kang Q, Ouyang S X, Ye J H 2014 ACS Nano 8 7078

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    Stephenson T, Li Z, Olsen B, Mitlin D 2014 Energy Environ. Sci. 7 209

    [11]

    Zhu C B, Mu X K, van Aken P A, Yu Y, Maier J 2014 Angew. Chem. Int. Ed. 53 2152

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    Deng D H, Fu Q, Novoselov K S, Fu Q, Zheng N F, Tian Z Q, Bao X H 2016 Nat. Nanotechnol. 11 218

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    Asadi M, Kumar B, Liu C, Phillips P, Yasaei P, Behranginia A, Zapol P, Klie R F, Curss L A, Salehi-Khojin A 2016 ACS Nano 10 2167

    [14]

    Yuwen L H, Xu F, Xue B, Luo Z M, Zhang Q, Bao B Q, Su S, Weng L X, Huang W, Wang L H 2014 Nanoscale 6 5762

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    Huang H, Feng X, Du C C, Wu S Y, Song W B 2015 J. Mater. Chem. A 3 16050

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    Gordon R B, Bertram M, Graedel T E 2006 Proc. Natl. Acad. Sci. USA 103 1209

    [17]

    Kong D, Wang H, Cha J J, Pasta M, Koski K J, Yao J, Cui Y 2013 Nano Lett. 13 1341

    [18]

    Ramakrishna Matte H S S, Gomathi A, Manna A K, Late D J, Datta R, Pati S K, Rao C N R 2010 Angew. Chem. Int. Ed. 49 4059

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    Laursen A B, Kegnæs S, Dahl S, Chorkendorff I 2012 Energy Environ. Sci. 5 5577

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    Merki D, Hu X L 2011 Energy Environ. Sci. 4 3878

    [21]

    Tang H, Dou K P, Kaun C C, Kuang Q, Yang S H 2014 J. Mater. Chem. A 2 360

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    Jaramillo T F, Jorgensen K P, Bonde J, Nielsen J H, Horch S, Chorkendorff I 2007 Science 317 100

    [23]

    Hinnemann B, Moses P G, Bonde J, Jørgensen K P, Nielsen J H, Horch S, Chorkendorff I B, Nørskov J K 2005 J. Am. Chem. Soc. 127 5308

    [24]

    Shu H B, Zhou D, Li F, Cao D, Chen X S 2017 ACS Appl. Mater. Interfaces 9 42688

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    Li Y, Wang H, Xie L, Liang Y, Hong G, Dai H 2011 J. Am. Chem. Soc. 133 7296

    [26]

    Xie J, Zhang H, Li S, Wang R, Sun X, Zhou M, Zhou J, Lou X W D, Xie, Y 2013 Adv. Mater. 25 5807

    [27]

    Voiry D, Salehi M, Silva R, Fujita T, Chen M W, Asefa T, Shenoy V B, Eda G, Chhowalla M 2013 Nano Lett. 13 6222

    [28]

    Lukowski M A, Daniel A S, Meng F, Forticaux A, Li L, Jin S 2013 J. Am. Chem. Soc. 135 10274

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    Eftekhari A 2017 Appl. Mater. Today 8 1

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    Hohenberg P, Kohn W 1964 Phys. Rev. 136 B864

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    Kohn W, Sham L 1965 Phys. Rev. 140 A1133

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    Kresse G, Hafner J 1994 Phys. Rev. B 49 14251

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    Kresse G Furthmller J 1996 Comput. Mater. Sci. 6 15

    [34]

    Liu L L, Li X Y, Xu L C, Liu R P, Yang Z 2017 J. Taiyuan Univ. Technol. 48 570 (in Chinese)[刘丽丽, 李秀燕, 徐利春, 刘瑞萍, 杨致 2017 太原理工大学学报 48 570]

    [35]

    Greeley J, Jaramillo T F, Bonde J, Chorkendorff I, Nørskov J K 2006 Nat. Mater. 5 909

    [36]

    Reuter K, Scheffler M 2001 Phys. Rev. B 65 035406

    [37]

    Kresse G, Hafner J 1993 Phys. Rev. B 47 558

    [38]

    Zheng Y, Jiao Y, Jaronice M, Qiao S Z 2015 Angew. Chem. Int. Ed. 54 52

    [39]

    Noerskov J K, Bligaard T, Logadottir A, Kitchin J R, Chen J G, Pandelov S, Stimming U 2005 J. ElectroChem. Soc. 152 J23

    [40]

    Wang B B, Zhu G, Wang Q 2016 Acta Phys. Sin. 65 038102 (in Chinese)[王必本, 朱恪, 王强 2016 物理学报 65 038102]

    [41]

    Tsai C, Chan K, Abild-Pedersen F, Nørskov J K 2014 Phys. Chem. Chem. Phys. 16 13156

    [42]

    Qu B, Yu X B, Chen Y J, Zhu C L, Li C Y, Yin Z X, Zhang X T 2015 ACS Appl. Mater. Interfaces 7 14170

    [43]

    Cui P, Choi J H, Chen W, Zeng J, Shih C K, Li Z Y, Zhang Z Y 2017 Nano Lett. 17 1097

    [44]

    Yang H X, Yan X R, Cui J Z, Wang J H, Wang X R, Qin X 2002 Inorganic Chemistry (Vol. 4) (Beijing: Higher Education Press) pp138-145 (in Chinese)[杨宏孝, 颜秀茹, 崔建中, 王建辉, 王兴尧, 秦学 2002 无机化学 (第四版) (北京: 高等教育出版社) 第138–145页]

    [45]

    Chen Y, Cui P, Ren X B, Zhang C D, Jin C H, Zhang Z Y, Shih C K 2017 Nat. Commun. 8 15135

  • [1]

    Wang Q H, Kalantar-Zadeh K, Kis A, Coleman J N, Strano M S 2012 Nat. Nanotechnol. 7 699

    [2]

    Radisavljevic B, Radenovic A, Brivio J, Giacometti I V, Kis A 2011 Nat. Nanotechnol. 6 147

    [3]

    Chhowalla M, Shin H S, Eda G, Li L J, Loh K P, Zhang H 2013 Nat. Chem. 5 263

    [4]

    Frame F A, Osterloh F E 2010 J. Phys. Chem. C 114 10628

    [5]

    Huang M, Cho K 2009 J. Phys. Chem. C 113 5238

    [6]

    Liu Z K, Lau S P, Yan F 2015 Chem. Soc. Rev. 44 5638

    [7]

    Xiang Q J, Yu J G, Jaroniec M 2012 J. Am. Chem. Soc. 134 6575

    [8]

    Ding Q, Meng F, English C R, Caban-Acevedo M, Shearer M J, Liang D, Daniel A S, Hamers R J, Jin S 2014 J. Am. Chem. Soc. 136 8504

    [9]

    Chang K, Mei Z W, Wang T, Kang Q, Ouyang S X, Ye J H 2014 ACS Nano 8 7078

    [10]

    Stephenson T, Li Z, Olsen B, Mitlin D 2014 Energy Environ. Sci. 7 209

    [11]

    Zhu C B, Mu X K, van Aken P A, Yu Y, Maier J 2014 Angew. Chem. Int. Ed. 53 2152

    [12]

    Deng D H, Fu Q, Novoselov K S, Fu Q, Zheng N F, Tian Z Q, Bao X H 2016 Nat. Nanotechnol. 11 218

    [13]

    Asadi M, Kumar B, Liu C, Phillips P, Yasaei P, Behranginia A, Zapol P, Klie R F, Curss L A, Salehi-Khojin A 2016 ACS Nano 10 2167

    [14]

    Yuwen L H, Xu F, Xue B, Luo Z M, Zhang Q, Bao B Q, Su S, Weng L X, Huang W, Wang L H 2014 Nanoscale 6 5762

    [15]

    Huang H, Feng X, Du C C, Wu S Y, Song W B 2015 J. Mater. Chem. A 3 16050

    [16]

    Gordon R B, Bertram M, Graedel T E 2006 Proc. Natl. Acad. Sci. USA 103 1209

    [17]

    Kong D, Wang H, Cha J J, Pasta M, Koski K J, Yao J, Cui Y 2013 Nano Lett. 13 1341

    [18]

    Ramakrishna Matte H S S, Gomathi A, Manna A K, Late D J, Datta R, Pati S K, Rao C N R 2010 Angew. Chem. Int. Ed. 49 4059

    [19]

    Laursen A B, Kegnæs S, Dahl S, Chorkendorff I 2012 Energy Environ. Sci. 5 5577

    [20]

    Merki D, Hu X L 2011 Energy Environ. Sci. 4 3878

    [21]

    Tang H, Dou K P, Kaun C C, Kuang Q, Yang S H 2014 J. Mater. Chem. A 2 360

    [22]

    Jaramillo T F, Jorgensen K P, Bonde J, Nielsen J H, Horch S, Chorkendorff I 2007 Science 317 100

    [23]

    Hinnemann B, Moses P G, Bonde J, Jørgensen K P, Nielsen J H, Horch S, Chorkendorff I B, Nørskov J K 2005 J. Am. Chem. Soc. 127 5308

    [24]

    Shu H B, Zhou D, Li F, Cao D, Chen X S 2017 ACS Appl. Mater. Interfaces 9 42688

    [25]

    Li Y, Wang H, Xie L, Liang Y, Hong G, Dai H 2011 J. Am. Chem. Soc. 133 7296

    [26]

    Xie J, Zhang H, Li S, Wang R, Sun X, Zhou M, Zhou J, Lou X W D, Xie, Y 2013 Adv. Mater. 25 5807

    [27]

    Voiry D, Salehi M, Silva R, Fujita T, Chen M W, Asefa T, Shenoy V B, Eda G, Chhowalla M 2013 Nano Lett. 13 6222

    [28]

    Lukowski M A, Daniel A S, Meng F, Forticaux A, Li L, Jin S 2013 J. Am. Chem. Soc. 135 10274

    [29]

    Eftekhari A 2017 Appl. Mater. Today 8 1

    [30]

    Hohenberg P, Kohn W 1964 Phys. Rev. 136 B864

    [31]

    Kohn W, Sham L 1965 Phys. Rev. 140 A1133

    [32]

    Kresse G, Hafner J 1994 Phys. Rev. B 49 14251

    [33]

    Kresse G Furthmller J 1996 Comput. Mater. Sci. 6 15

    [34]

    Liu L L, Li X Y, Xu L C, Liu R P, Yang Z 2017 J. Taiyuan Univ. Technol. 48 570 (in Chinese)[刘丽丽, 李秀燕, 徐利春, 刘瑞萍, 杨致 2017 太原理工大学学报 48 570]

    [35]

    Greeley J, Jaramillo T F, Bonde J, Chorkendorff I, Nørskov J K 2006 Nat. Mater. 5 909

    [36]

    Reuter K, Scheffler M 2001 Phys. Rev. B 65 035406

    [37]

    Kresse G, Hafner J 1993 Phys. Rev. B 47 558

    [38]

    Zheng Y, Jiao Y, Jaronice M, Qiao S Z 2015 Angew. Chem. Int. Ed. 54 52

    [39]

    Noerskov J K, Bligaard T, Logadottir A, Kitchin J R, Chen J G, Pandelov S, Stimming U 2005 J. ElectroChem. Soc. 152 J23

    [40]

    Wang B B, Zhu G, Wang Q 2016 Acta Phys. Sin. 65 038102 (in Chinese)[王必本, 朱恪, 王强 2016 物理学报 65 038102]

    [41]

    Tsai C, Chan K, Abild-Pedersen F, Nørskov J K 2014 Phys. Chem. Chem. Phys. 16 13156

    [42]

    Qu B, Yu X B, Chen Y J, Zhu C L, Li C Y, Yin Z X, Zhang X T 2015 ACS Appl. Mater. Interfaces 7 14170

    [43]

    Cui P, Choi J H, Chen W, Zeng J, Shih C K, Li Z Y, Zhang Z Y 2017 Nano Lett. 17 1097

    [44]

    Yang H X, Yan X R, Cui J Z, Wang J H, Wang X R, Qin X 2002 Inorganic Chemistry (Vol. 4) (Beijing: Higher Education Press) pp138-145 (in Chinese)[杨宏孝, 颜秀茹, 崔建中, 王建辉, 王兴尧, 秦学 2002 无机化学 (第四版) (北京: 高等教育出版社) 第138–145页]

    [45]

    Chen Y, Cui P, Ren X B, Zhang C D, Jin C H, Zhang Z Y, Shih C K 2017 Nat. Commun. 8 15135

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出版历程
  • 收稿日期:  2018-05-04
  • 修回日期:  2018-09-05
  • 刊出日期:  2018-11-05

电化学析氢反应中单层MoSe2氢吸附机理第一性原理研究

    基金项目: 

    国家自然科学基金(批准号:11774136,11404144)、中国博士后科学基金(批准号:2016M601722,2018T110445)和江苏大学科研基金(批准号:14JDG120)资助的课题.

摘要: 基于密度泛函理论的第一性原理方法,本文计算了单层2H相MoSe2纳米材料表面及两种边缘(Mo原子边缘、Se原子边缘)不同活性位点、不同氢原子吸附率下的氢吸附吉布斯自由能(Gibbs free energy,用△GH0表示),并且将对应的微观结构进行了系统分析比较,得出△GH0最接近于0 eV的吸附位点及相应的吸附率.同时,结合差分电荷密度和电负性理论,分析了单层MoSe2两种边缘氢吸附的电荷转移及成键特性,进一步解释了不同吸附位点呈现的结构与能量趋势.最后,通过基于密度泛函理论的第一性原理分子动力学模拟,研究了高温热运动对两种边缘氢吸附的影响,获得了氢原子发生脱附的临界温度及对应的微观动态过程.该理论研究从原子尺度揭示了单层2H相MoSe2纳米材料边缘不同位点在不同温度下对氢原子吸附和脱附的微观机理,证实了Mo原子边缘的畸变和重构行为,加深了对实验中单层2H相MoSe2边缘在不同温度下氢吸附机理的理解,为实验中通过控制MoSe2边缘设计廉价高效的析氢催化剂提供理论参考.

English Abstract

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