Volume 8 Issue 4
Aug.  2023
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Article Navigation >  Green Energy&Environment  > 2023  >  8(4): 1185-1194
Mengzhao Zhang, Hanqing Yin, Fuhao Jin, Jingquan Liu, Xuqiang Ji, Aijun Du, Wenrong Yang, Zhen Liu. Vacancy engineering of oxidized Nb2CTx MXenes for a biased nitrogen fixation. Green Energy&Environment, 2023, 8(4): 1185-1194. doi: 10.1016/j.gee.2022.01.010
Citation: Mengzhao Zhang, Hanqing Yin, Fuhao Jin, Jingquan Liu, Xuqiang Ji, Aijun Du, Wenrong Yang, Zhen Liu. Vacancy engineering of oxidized Nb2CTx MXenes for a biased nitrogen fixation. Green Energy&Environment, 2023, 8(4): 1185-1194. doi: 10.1016/j.gee.2022.01.010
shu

Vacancy engineering of oxidized Nb2CTx MXenes for a biased nitrogen fixation

doi: 10.1016/j.gee.2022.01.010

  • a. College of Materials Science and Engineering, Institute for Graphene Applied Technology Innovation, Qingdao University, 308 Ningxia Road, Qingdao, 266071, China;

  • b. School of Chemistry and Physics and Centre for Materials Science, Queensland University of Technology, Gardens Point Campus, Brisbane, 4001, Australia;

  • c. School of Life and Environmental Sciences, Deakin University, 75 Pigdons Road, Geelong, VIC 3216, Australia

Funds:

This work was financially supported by China Postdoctoral Science Foundation (2019M652305) and Qingdao Postdoctoral Application Research Project. A. Du acknowledges the support of high-performance computer resources provided by NCI National Facility and The Pawsey Supercomputing Centre through the National Computational Merit Allocation Scheme provided by the Australian Government and the Government of Western Australia.

  • Received date 04 October 2021, Accepted date 18 January 2022, RevRecd date 04 January 2022, Available online 07 July 2023, Publish date 24 January 2022,
    Abstract
  • The artificial nitrogen (N2) reduction reaction (NRR) via electrocatalysis is a newly developed methodology to produce ammonia (NH3) at ambient conditions, but faces the challenges in N2 activation and poor reaction selectivity. Herein, Nb-based MXenes are developed to remarkably enhance the NRR activity through the engineering of the stretched 3D structure and oxygen vacancies (VO). The theoretical studies indicate that N2 could be initially adsorbed on VO with an end-on configuration, and the potential determining step might be the first hydrogenation step. The catalysts achieve an NH3 production rate of 29.1 μg h-1 mgcat-1 and excellent Faradic efficiency of 11.5%, surpassing other Nb-based catalysts. The selectivity of NRR is assigned to the unique structure of the catalysts, including (1) the layered graphitic structure for fast electron transfer and active site distribution, (2) the reactive VO for N2 adsorption and activation, and (3) the expanded interlayer space for mass transfer.

     

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    • References(63)
  • [1]
    K.A. Brown, D.F. Harris, M.B. Wilker, A. Rasmussen, N. Khadka, H. Hamby, S. Keable, G. Dukovic, J.W. Peters, L.C. Seefeldt, P.W. King, Science 352 (2016) 448-450.
    [2]
    J.G. Chen, R.M. Crooks, L.C. Seefeldt, K.L. Bren, R.M. Bullock, M.Y. Darensbourg, P.L. Holland, B. Hoffman, M.J. Janik, A.K. Jones, M.G. Kanatzidis, P. King, K.M. Lancaster, S.V. Lymar, P. Pfromm, W.F. Schneider, R.R. Schrock, Science 360 (2018) eaar6611.
    [3]
    Y. Luo, G.-F. Chen, L. Ding, X. Chen, L.-X. Ding, H. Wang, Joule 3 (2019) 279-289.
    [4]
    X. Wu, L. Xia, Y. Wang, W. Lu, Q. Liu, X. Shi, X. Sun, Small 14 (2018) 1803111.
    [5]
    Y. Liu, Y. Su, X. Quan, X. Fan, S. Chen, H. Yu, H. Zhao, Y. Zhang, J. Zhao, ACS Catal. 8 (2018) 1186-1191.
    [6]
    Y. Zhang, W. Qiu, Y. Ma, Y. Luo, Z. Tian, G. Cui, F. Xie, L. Chen, T. Li, X. Sun, ACS Catal. 8 (2018) 8540-8544.
    [7]
    Z. Liu, M. Zhang, H. Wang, D. Cang, X. Ji, B. Liu, W. Yang, D. Li, J. Liu, ACS Sustain. Chem. Eng. 8 (2020) 5278-5286.
    [8]
    H. Zou, W. Rong, B. Long, Y. Ji, L. Duan, ACS Catal. 9 (2019) 10649-10655.
    [9]
    S. Zhang, X. Zhang, Y. Rui, R. Wang, X. Li, Green Energy Environ. 6 (2021) 458-478.
    [10]
    H.-M. Liu, S.-H. Han, Y. Zhao, Y.-Y. Zhu, X.-L. Tian, J.-H. Zeng, J.-X. Jiang, B.Y. Xia, Y. Chen, J. Mater. Chem. 6 (2018) 3211-3217.
    [11]
    D. Bao, Q. Zhang, F.-L. Meng, H.-X. Zhong, M.-M. Shi, Y. Zhang, J.-M. Yan, Q. Jiang, X.-B. Zhang, Adv. Mater. 29 (2017) 1604799.
    [12]
    J. Wang, L. Yu, L. Hu, G. Chen, H. Xin, X. Feng, Nat. Commun. 9 (2018) 1795.
    [13]
    S.-J. Li, D. Bao, M.-M. Shi, B.-R. Wulan, J.-M. Yan, Q. Jiang, Adv. Mater. 29 (2017) 1700001.
    [14]
    R. Zhang, X. Ren, X. Shi, F. Xie, B. Zheng, X. Guo, X. Sun, ACS Appl. Mater. Interfaces 10 (2018) 28251-28255.
    [15]
    P. Niu, T. Wu, L. Wen, J. Tan, Y. Yang, S. Zheng, Y. Liang, F. Li, J.T.S. Irvine, G. Liu, X. Ma, H.-M. Cheng, Adv. Mater. 30 (2018) 1705999.
    [16]
    Q. Zhang, W.-Z. Wang, J.-J. Yu, D.-H. Qu, H. Tian, Adv. Mater. 29 (2017) 1604948.
    [17]
    J. Han, Z. Liu, Y. Ma, G. Cui, F. Xie, F. Wang, Y. Wu, S. Gao, Y. Xu, X. Sun, Nano Energy 52 (2018) 264-270.
    [18]
    C.B. Li, D.W. Ma, S.Y. Mou, Y.S. Luo, B.Y. Ma, S.Y. Lu, G.W. Cui, Q. Li, Q. Liu, X.P. Sun, J. Energy Chem. 50 (2020) 402-408.
    [19]
    W.R. Liao, K. Xie, L.J. Liu, X.Y. Wang, Y. Luo, S.J. Liang, F.J. Liu, L.L. Jiang, J. Energy Chem. 62 (2021) 359-366.
    [20]
    Y. Fang, Z. Liu, J. Han, Z. Jin, Y. Han, F. Wang, Y. Niu, Y. Wu, Y. Xu, Adv. Energy Mater. 9 (2019) 1803406.
    [21]
    C.C. Leong, Y. Qu, Y. Kawazoe, S.K. Ho, H. Pan, Catal. Today 370 (2021) 2-13.
    [22]
    X. Li, Y. Luo, Q. Li, Y. Guo, K. Chu, J. Mater. Chem. 9 (2021) 15955-15962.
    [23]
    Z. Liu, J. Liu, D. Li, P.S. Francis, N.W. Barnett, C.J. Barrow, W. Yang, Chem. Commun. 51 (2015) 10969-10972.
    [24]
    Z. Liu, A. Dibaji, D. Li, S. Mateti, J. Liu, F. Yan, C.J. Barrow, Y. Chen, K. Ariga, W. Yang, Mater. Today 44 (2021) 194-210.
    [25]
    A. VahidMohammadi, J. Rosen, Y. Gogotsi, Science 372 (2021) .
    [26]
    J.-T. Ren, Y. Yao, Z.-Y. Yuan, Green Energy Environ. 6 (2021) 620-643.
    [27]
    Y. Wang, Y. Nian, A.N. Biswas, W. Li, Y. Han, J.G. Chen, Adv. Energy Mater. 11 (2021) 2002967.
    [28]
    B. Anasori, M.R. Lukatskaya, Y. Gogotsi, Nat. Rev. Mater. 2 (2017) 16098.
    [29]
    L.R. Johnson, S. Sridhar, L. Zhang, K.D. Fredrickson, A.S. Raman, J. Jang, C. Leach, A. Padmanabhan, C.C. Price, N.C. Frey, A. Raizada, V. Rajaraman, S.A. Saiprasad, X. Tang, A. Vojvodic, ACS Catal. 10 (2020) 253-264.
    [30]
    L. Ding, Y. Wei, L. Li, T. Zhang, H. Wang, J. Xue, L.-X. Ding, S. Wang, J. Caro, Y. Gogotsi, Nat. Commun. 9 (2018) 155.
    [31]
    M. Naguib, O. Mashtalir, M.R. Lukatskaya, B. Dyatkin, C.F. Zhang, V. Presser, Y. Gogotsi, M.W. Barsoum, Chem. Commun. 50 (2014) 7420-7423.
    [32]
    M. Naguib, O. Mashtalir, J. Carle, V. Presser, J. Lu, L. Hultman, Y. Gogotsi, M.W. Barsoum, ACS Nano 6 (2012) 1322-1331.
    [33]
    A. Ali, K. Hantanasirisakul, A. Abdala, P. Urbankowski, M.-Q. Zhao, B. Anasori, Y. Gogotsi, B. Aissa, K.A. Mahmoud, Langmuir 34 (2018) 11325-11334.
    [34]
    T.M. Su, R. Peng, Z.D. Hood, M. Naguib, I.N. Ivanov, J.K. Keum, Z.Z. Qin, Z.H. Guo, Z.L. Wu, ChemSusChem 11 (2018) 688-699.
    [35]
    D. Zhu, L.H. Zhang, R.E. Ruther, R.J. Hamers, Nat. Mater. 12 (2013) 836-841.
    [36]
    G. Kresse, J. Hafner, Phys. Rev. B 47 (1993) 558.
    [37]
    G. Kresse, D. Joubert, Phys. Rev. B 59 (1999) 1758.
    [38]
    J.P. Perdew, J.A. Chevary, S.H. Vosko, K.A. Jackson, M.R. Pederson, D.J. Singh, C. Fiolhais, Phys. Rev. B 46 (1992) 6671.
    [39]
    J.P. Perdew, Y. Wang, Phys. Rev. B 45 (1992) 13244.
    [40]
    J.K. Noerskov, J. Rossmeisl, A. Logadottir, L. Lindqvist, J.R. Kitchin, T. Bligaard, H. Jonsson, J. Phys. Chem. B 108 (2004) 17886-17892.
    [41]
    H. Hirakawa, M. Hashimoto, Y. Shiraishi, T. Hirai, J. Am. Chem. Soc. 139 (2017) 10929-10936.
    [42]
    C. Ling, Y. Ouyang, Q. Li, X. Bai, X. Mao, A. Du, J. Wang, Small Methods 3 (2019) 1800376.
    [43]
    S. Tang, Q. Dang, T. Liu, S. Zhang, Z. Zhou, X. Li, X. Wang, E. Sharman, Y. Luo, J. Jiang, J. Am. Chem. Soc. 142 (2020) 19308-19315.
    [44]
    J. Zhao, Z. Chen, J. Am. Chem. Soc. 139 (2017) 12480-12487.
    [45]
    W.Y. Yuan, L.F. Cheng, Y.N. Zhang, H. Wu, S.L. Lv, L.Y. Chai, X.H. Guo, L.X. Zheng, Adv. Mater. Interfac. 4 (2017) 11.
    [46]
    E. Pomerantseva, Y. Gogotsi, Nat. Energy 2 (2017) 17089.
    [47]
    Z.U.D. Babar, J. Fatheema, N. Arif, M.S. Anwar, S. Gul, M. Iqbal, S. Rizwan, RSC Adv. 10 (2020) 25669-25678.
    [48]
    C. Peng, P. Wei, X. Chen, Y.L. Zhang, F. Zhu, Y.H. Cao, H.J. Wang, H. Yu, F. Peng, Ceram. Int. 44 (2018) 18886-18893.
    [49]
    F. Shahzad, M. Alhabeb, C.B. Hatter, B. Anasori, S. Man Hong, C.M. Koo, Y. Gogotsi, Science 353 (2016) 1137-1140.
    [50]
    A. Lipatov, M. Alhabeb, M.R. Lukatskaya, A. Boson, Y. Gogotsi, A. Sinitskii, Adv. Electron. Mater. 2 (2016) 1600255.
    [51]
    C. Zhang, M. Beidaghi, M. Naguib, M.R. Lukatskaya, M.-Q. Zhao, B. Dyatkin, K.M. Cook, S.J. Kim, B. Eng, X. Xiao, D. Long, W. Qiao, B. Dunn, Y. Gogotsi, Chem. Mater. 28 (2016) 3937-3943.
    [52]
    Z. Yue, D. Chu, H. Huang, J. Huang, P. Yang, Y. Du, M. Zhu, C. Lu, RSC Adv. 5 (2015) 47117-47124.
    [53]
    S.W. Song, J.Q. Liu, C.L. Zhou, Q. Jia, H. Luo, L.W. Deng, X.X. Wang, J. Alloys Compd. 843 (2020) 9.
    [54]
    H. Lin, S. Gao, C. Dai, Y. Chen, J. Shi, J. Am. Chem. Soc. 139 (2017) 16235-16247.
    [55]
    W.L. Zhang, J.M. Tian, H.B. Zeng, J.Q. Liu, Y. Tian, Chem. Eng. J. 366 (2019) 321-329.
    [56]
    M. Naguib, J. Halim, J. Lu, K.M. Cook, L. Hultman, Y. Gogotsi, M.W. Barsoum, J. Am. Chem. Soc. 135 (2013) 15966-15969.
    [57]
    C.E. Ren, M.Q. Zhao, T. Makaryan, J. Halim, M. Boota, S. Kota, B. Anasori, M.W. Barsoum, Y. Gogotsi, Chemelectrochem 3 (2016) 689-693.
    [58]
    C.F. Shi, K.X. Xiang, Y.R. Zhu, X.H. Chen, W. Zhou, H. Chen, Electrochim. Acta 246 (2017) 1088-1096.
    [59]
    J. Kibsgaard, C. Tsai, K. Chan, J.D. Benck, J.K. Norskov, F. Abild-Pedersen, T.F. Jaramillo, Energy Environ. Sci. 8 (2015) 3022-3029.
    [60]
    X. Yu, P. Han, Z. Wei, L. Huang, Z. Gu, S. Peng, J. Ma, G. Zheng, Joule 2 (2018) 1610-1622.
    [61]
    W. Qiu, X.-Y. Xie, J. Qiu, W.-H. Fang, R. Liang, X. Ren, X. Ji, G. Cui, A.M. Asiri, G. Cui, B. Tang, X. Sun, Nat. Commun. 9 (2018) 3485.
    [62]
    J. Kong, A. Lim, C. Yoon, J.H. Jang, H.C. Ham, J. Han, S. Nam, D. Kim, Y.-E. Sung, J. Choi, H.S. Park, ACS Sustain. Chem. Eng. 5 (2017) 10986-10995.
    [63]
    G. Watt, J. Chrisp, Clin. Chim. Acta 26 (1954) 452-453.
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