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

Howard Yi Fan Sim; Jaslyn Ru Ting Chen; Charlynn Sher Lin Koh; Hiang Kwee Lee; Xuemei Han; Gia Chuong Phan-Quang; Jing Yi Pang; Chee Leng Lay; Srikanth Pedireddy; In Yee Phang; Edwin Kok Lee Yeow; Xing Yi Ling

doi:10.1002/anie.202006071

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

Howard Yi Fan Sim, Jaslyn Ru Ting Chen, Charlynn Sher Lin Koh, Hiang Kwee Lee, Xuemei Han, Gia Chuong Phan-Quang, Jing Yi Pang, Chee Leng Lay, Srikanth Pedireddy, In Yee Phang, Edwin Kok Lee Yeow, Xing Yi Ling

Biological, Environmental Sciences and Engineering

Research output: Contribution to journal › Article › peer-review

132 Scopus citations

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.

Original language	English (US)
Journal	Angewandte Chemie (International ed. in English)
DOIs	https://doi.org/10.1002/anie.202006071
State	Published - May 29 2020

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: 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.

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https://repository.kaust.edu.sa/bitstream/10754/662985/1/ZIF_anie.202006071.pdf

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Sim, H. Y. F., Chen, J. R. T., Koh, C. S. L., Lee, H. K., Han, X., Phan-Quang, G. C., Pang, J. Y., Lay, C. L., Pedireddy, S., Phang, I. Y., Yeow, E. K. L., & Ling, X. Y. (2020). ZIF-induced d-band Modification in Bimetallic Nanocatalyst: Achieving >44% Efficiency in Ambient Nitrogen Reduction Reaction. Angewandte Chemie (International ed. in English). https://doi.org/10.1002/anie.202006071

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

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.",

author = "Sim, {Howard Yi Fan} and Chen, {Jaslyn Ru Ting} and Koh, {Charlynn Sher Lin} and Lee, {Hiang Kwee} and Xuemei Han and Phan-Quang, {Gia Chuong} and Pang, {Jing Yi} and Lay, {Chee Leng} and Srikanth Pedireddy and Phang, {In Yee} and Yeow, {Edwin Kok Lee} and Ling, {Xing Yi}",

note = "KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: 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.",

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doi = "10.1002/anie.202006071",

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AU - Sim, Howard Yi Fan

AU - Chen, Jaslyn Ru Ting

AU - Koh, Charlynn Sher Lin

AU - Lee, Hiang Kwee

AU - Han, Xuemei

AU - Phan-Quang, Gia Chuong

AU - Pang, Jing Yi

AU - Lay, Chee Leng

AU - Pedireddy, Srikanth

AU - Phang, In Yee

AU - Yeow, Edwin Kok Lee

AU - Ling, Xing Yi

N1 - KAUST Repository Item: Exported on 2020-10-01 Acknowledgements: 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.

PY - 2020/5/29

Y1 - 2020/5/29

N2 - 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.

AB - 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.

UR - http://hdl.handle.net/10754/662985

UR - https://onlinelibrary.wiley.com/doi/abs/10.1002/anie.202006071

U2 - 10.1002/anie.202006071

DO - 10.1002/anie.202006071

M3 - Article

C2 - 32463536

SN - 1433-7851

JO - Angewandte Chemie (International ed. in English)

JF - Angewandte Chemie (International ed. in English)

ER -

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

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