Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

Lili Han; Xijun Liu; Jinping Chen; Ruoqian Lin; Haoxuan Liu; L. U. Fang; Seongmin Bak; Zhixiu Liang; Shunzheng Zhao; Eli Stavitski; Jun Luo; Radoslav R. Adzic; Huolin L. Xin

doi:10.1002/anie.201811728

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

Lili Han, Xijun Liu, Jinping Chen, Ruoqian Lin, Haoxuan Liu, L. U. Fang, Seongmin Bak, Zhixiu Liang, Shunzheng Zhao, Eli Stavitski, Jun Luo, Radoslav R. Adzic, Huolin L. Xin

Department of Materials Science and Engineering

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

Abstract

NH ₃ synthesis by the electrocatalytic N ₂ reduction reaction (NRR) under ambient conditions is an appealing alternative to the currently employed industrial method—the Haber–Bosch process—that requires high temperature and pressure. We report single Mo atoms anchored to nitrogen-doped porous carbon as a cost-effective catalyst for the NRR. Benefiting from the optimally high density of active sites and hierarchically porous carbon frameworks, this catalyst achieves a high NH ₃ yield rate (34.0±3.6 μg _NH3 h ⁻¹ mg _cat. ⁻¹ ) and a high Faradaic efficiency (14.6±1.6 %) in 0.1 m KOH at room temperature. These values are considerably higher compared to previously reported non-precious-metal electrocatalysts. Moreover, this catalyst displays no obvious current drop during a 50 000 s NRR, and high activity and durability are achieved in 0.1 m HCl. The findings provide a promising lead for the design of efficient and robust single-atom non-precious-metal catalysts for the electrocatalytic NRR.

Original language	English
Pages (from-to)	2321-2325
Number of pages	5
Journal	Angewandte Chemie - International Edition
Volume	58
Issue number	8
DOIs	https://doi.org/10.1002/anie.201811728
Publication status	Published - 2019 Feb 18

Bibliographical note

Funding Information:
This work was financially supported by National Key R&D Program of China (2017YFA0700104), National Natural Science Foundation of China (21601136 and 51761165012), National Program for Thousand Young Talents of China, Tianjin Municipal Science and Technology Commission (15JCYBJC52600), Tianjin Municipal Education Commission, and the Fundamental Research Fund of Tianjin University of Technology. This research used resources of the National Synchrotron Light Source II and the Center for Functional Nanomaterials, U.S. Department of Energy (DOE) Office of Science User Facilities operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. S.B. was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the US Department of Energy through the Advanced Battery Materials Research (BMR) Program, including the Battery500 Consortium under contract DE-SC0012704 with the U.S. Department of Energy. The work by Z.L. and R.R.A. was supported by the Division of Chemical Sciences, Geosciences, & Biosciences, Office of Basic Energy Sciences and carried out under Contract No. DE-SC0012704 with the U.S. Department of Energy.

Publisher Copyright:
© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

All Science Journal Classification (ASJC) codes

Catalysis
Chemistry(all)

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10.1002/anie.201811728

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@article{74410ee88699457695ffd9a5fb5bc67c,

title = "Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation",

abstract = " NH 3 synthesis by the electrocatalytic N 2 reduction reaction (NRR) under ambient conditions is an appealing alternative to the currently employed industrial method—the Haber–Bosch process—that requires high temperature and pressure. We report single Mo atoms anchored to nitrogen-doped porous carbon as a cost-effective catalyst for the NRR. Benefiting from the optimally high density of active sites and hierarchically porous carbon frameworks, this catalyst achieves a high NH 3 yield rate (34.0±3.6 μg NH3 h −1 mg cat. −1 ) and a high Faradaic efficiency (14.6±1.6 %) in 0.1 m KOH at room temperature. These values are considerably higher compared to previously reported non-precious-metal electrocatalysts. Moreover, this catalyst displays no obvious current drop during a 50 000 s NRR, and high activity and durability are achieved in 0.1 m HCl. The findings provide a promising lead for the design of efficient and robust single-atom non-precious-metal catalysts for the electrocatalytic NRR.",

author = "Lili Han and Xijun Liu and Jinping Chen and Ruoqian Lin and Haoxuan Liu and Fang, {L. U.} and Seongmin Bak and Zhixiu Liang and Shunzheng Zhao and Eli Stavitski and Jun Luo and Adzic, {Radoslav R.} and Xin, {Huolin L.}",

note = "Funding Information: This work was financially supported by National Key R&D Program of China (2017YFA0700104), National Natural Science Foundation of China (21601136 and 51761165012), National Program for Thousand Young Talents of China, Tianjin Municipal Science and Technology Commission (15JCYBJC52600), Tianjin Municipal Education Commission, and the Fundamental Research Fund of Tianjin University of Technology. This research used resources of the National Synchrotron Light Source II and the Center for Functional Nanomaterials, U.S. Department of Energy (DOE) Office of Science User Facilities operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. S.B. was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the US Department of Energy through the Advanced Battery Materials Research (BMR) Program, including the Battery500 Consortium under contract DE-SC0012704 with the U.S. Department of Energy. The work by Z.L. and R.R.A. was supported by the Division of Chemical Sciences, Geosciences, & Biosciences, Office of Basic Energy Sciences and carried out under Contract No. DE-SC0012704 with the U.S. Department of Energy. Publisher Copyright: {\textcopyright} 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim",

year = "2019",

month = feb,

day = "18",

doi = "10.1002/anie.201811728",

language = "English",

volume = "58",

pages = "2321--2325",

journal = "Angewandte Chemie - International Edition",

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T1 - Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

AU - Han, Lili

AU - Liu, Xijun

AU - Chen, Jinping

AU - Lin, Ruoqian

AU - Liu, Haoxuan

AU - Fang, L. U.

AU - Bak, Seongmin

AU - Liang, Zhixiu

AU - Zhao, Shunzheng

AU - Stavitski, Eli

AU - Luo, Jun

AU - Adzic, Radoslav R.

AU - Xin, Huolin L.

N1 - Funding Information: This work was financially supported by National Key R&D Program of China (2017YFA0700104), National Natural Science Foundation of China (21601136 and 51761165012), National Program for Thousand Young Talents of China, Tianjin Municipal Science and Technology Commission (15JCYBJC52600), Tianjin Municipal Education Commission, and the Fundamental Research Fund of Tianjin University of Technology. This research used resources of the National Synchrotron Light Source II and the Center for Functional Nanomaterials, U.S. Department of Energy (DOE) Office of Science User Facilities operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. S.B. was supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the US Department of Energy through the Advanced Battery Materials Research (BMR) Program, including the Battery500 Consortium under contract DE-SC0012704 with the U.S. Department of Energy. The work by Z.L. and R.R.A. was supported by the Division of Chemical Sciences, Geosciences, & Biosciences, Office of Basic Energy Sciences and carried out under Contract No. DE-SC0012704 with the U.S. Department of Energy. Publisher Copyright: © 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

PY - 2019/2/18

Y1 - 2019/2/18

N2 - NH 3 synthesis by the electrocatalytic N 2 reduction reaction (NRR) under ambient conditions is an appealing alternative to the currently employed industrial method—the Haber–Bosch process—that requires high temperature and pressure. We report single Mo atoms anchored to nitrogen-doped porous carbon as a cost-effective catalyst for the NRR. Benefiting from the optimally high density of active sites and hierarchically porous carbon frameworks, this catalyst achieves a high NH 3 yield rate (34.0±3.6 μg NH3 h −1 mg cat. −1 ) and a high Faradaic efficiency (14.6±1.6 %) in 0.1 m KOH at room temperature. These values are considerably higher compared to previously reported non-precious-metal electrocatalysts. Moreover, this catalyst displays no obvious current drop during a 50 000 s NRR, and high activity and durability are achieved in 0.1 m HCl. The findings provide a promising lead for the design of efficient and robust single-atom non-precious-metal catalysts for the electrocatalytic NRR.

AB - NH 3 synthesis by the electrocatalytic N 2 reduction reaction (NRR) under ambient conditions is an appealing alternative to the currently employed industrial method—the Haber–Bosch process—that requires high temperature and pressure. We report single Mo atoms anchored to nitrogen-doped porous carbon as a cost-effective catalyst for the NRR. Benefiting from the optimally high density of active sites and hierarchically porous carbon frameworks, this catalyst achieves a high NH 3 yield rate (34.0±3.6 μg NH3 h −1 mg cat. −1 ) and a high Faradaic efficiency (14.6±1.6 %) in 0.1 m KOH at room temperature. These values are considerably higher compared to previously reported non-precious-metal electrocatalysts. Moreover, this catalyst displays no obvious current drop during a 50 000 s NRR, and high activity and durability are achieved in 0.1 m HCl. The findings provide a promising lead for the design of efficient and robust single-atom non-precious-metal catalysts for the electrocatalytic NRR.

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U2 - 10.1002/anie.201811728

DO - 10.1002/anie.201811728

M3 - Article

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AN - SCOPUS:85060243358

SN - 1433-7851

VL - 58

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EP - 2325

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 8

ER -

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

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