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    ZIF-induced d-band Modification in Bimetallic Nanocatalyst: Achieving >44% Efficiency in Ambient Nitrogen Reduction Reaction.

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    ZIF_anie.202006071.pdf
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    Description:
    Accepted manuscript
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    Type
    Article
    Authors
    Sim, Howard Yi Fan
    Chen, Jaslyn Ru Ting
    Koh, Charlynn Sher Lin
    Lee, Hiang Kwee
    Han, Xuemei
    Phan-Quang, Gia Chuong
    Pang, Jing Yi
    Lay, Chee Leng
    Pedireddy, Srikanth cc
    Phang, In Yee
    Yeow, Edwin Kok Lee
    Ling, Xing Yi
    KAUST Department
    Biological and Environmental Sciences and Engineering (BESE) Division
    Water Desalination and Reuse Research Center (WDRC)
    Date
    2020-07-27
    Online Publication Date
    2020-07-27
    Print Publication Date
    2020-09-21
    Embargo End Date
    2021-05-29
    Submitted Date
    2020-04-27
    Permanent link to this record
    http://hdl.handle.net/10754/662985
    
    Metadata
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    Abstract
    Electrochemical nitrogen reduction reaction (NRR) offers a sustainable solution towards ammonia production but suffers poor reaction performance due to preferential catalyst-H formation and the consequential hydrogen evolution reaction (HER). Herein, we electronically modify PtAu electrocatalyst d-band structure using zeolitic-imidazole framework (ZIF) to achieve a faradaic efficiency (FE) of >44% with high ammonia yield rate of >161 µg.mg cat -1 .h -1 at ambient conditions. Our strategy lowers electrocatalyst d-band position to weaken H adsorption and concurrently creates electron deficient sites to kinetically drive NRR by promoting catalyst-N 2 interaction. The ZIF coating on electrocatalyst doubles as a hydrophobic layer to suppress HER, further improves FE by >44-fold compared to without ZIF (~1%). Experimental and in-silico studies reveal PtAu-N ZIF interaction is key to enable strong N 2 adsorption over H atom. Our electrocatalytic design is universal and can be extended across metal electrocatalysts for diverse applications in NRR and air-to-fuel conversion.
    Citation
    Sim, H. Y. F., Chen, J. R. T., Koh, C. S. L., Lee, H. K., Han, X., Phan-Quang, G. C., … Ling, X. Y. (2020). ZIF-induced d-band Modification in Bimetallic Nanocatalyst: Achieving >44% Efficiency in Ambient Nitrogen Reduction Reaction. Angewandte Chemie International Edition. doi:10.1002/anie.202006071
    Sponsors
    This research is supported by the Ministry of Education, Singapore, under Tier 1 (RG11/18) and Tier 2 (MOE2016-T2-1-043) grants, and Max Planck Institute-Nanyang Technological University Joint Lab. H. Y. F. S., C. S. L. K. and G. C. P-Q. thank scholarship support from Nanyang Technological University, Singapore. J. R. T. C. and J. Y. P. thank CN Yang scholarship. H. K. L. thanks the International Postdoctoral Scholarship support from Nanyang Technological University, Singapore, and Singapore Ministry of Education. We thank Mr. Poh Chong Lim, A*STAR, for XRD analysis.
    Publisher
    Wiley
    Journal
    Angewandte Chemie
    DOI
    10.1002/anie.202006071
    PubMed ID
    32463536
    Additional Links
    https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202006071
    ae974a485f413a2113503eed53cd6c53
    10.1002/anie.202006071
    Scopus Count
    Collections
    Articles; Biological and Environmental Science and Engineering (BESE) Division; Water Desalination and Reuse Research Center (WDRC)

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