Element-dependent effects of alkali cations on nitrate reduction to ammonia

Yida Zhang ¹Zhentao Ma ²Shaokang Yang ³Qingyu Wang ¹Limin Liu ²Yu Bai ⁴Dewei Rao ³Gongming Wang ⁴Hongliang Li ⁵Xusheng Zheng²

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作者信息

1. National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230029,China;College of Chemistry and Materials Science,Experimental Center of Engineering and Material Science,University of Science and Technology of China,Hefei 230026,China
2. National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230029,China
3. School of Materials Science and Engineering,Jiangsu University,Zhenjiang 212013,China
4. College of Chemistry and Materials Science,Experimental Center of Engineering and Material Science,University of Science and Technology of China,Hefei 230026,China
5. National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230029,China;Hefei National Research Center for Physical Sciences at the Microscale,University of Science and Technology of China,Hefei 230026,China
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Abstract

Catalytic conversion of nitrate(NO3-)pollutants into ammonia(NH3)offers a sustainable and promising route for both wastewater treatment and NH3 synthesis.Alkali cations are prevalent in nitrate solutions,but their roles beyond charge balance in catalytic NO3 conversion have been generally ignored.Herein,we report the promotion effect of K+cations in KNO3 solution for NO3-reduction over a TiO2-supported Ni single-atom catalyst(Ni1/TiO2).For photocatalytic NO3-reduction reaction,Ni1/TiO2 exhib-ited a 1.9-fold NH3 yield rate with nearly 100％selectivity in KNO3 solution relative to that in NaNO3 solu-tion.Mechanistic studies reveal that the K+cations from KNO3 gradually bonded with the surface of Ni1/TiO2,in situ forming a K-O-Ni moiety during reaction,whereas the Na+ions were unable to interact with the catalyst in NaNO3 solution.The charge accumulation on the Ni sites induced by the incorporation of K atom promoted the adsorption and activation of NO3-.Furthermore,the K-O-Ni moiety facilitated the multiple proton-electron coupling of NO3 into NH3 by stabilizing the intermediates.

Key words

Nitrate reduction/Alkali cations/Potassium/Ni single-atom catalyst/Ammonia

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基金项目

National Natural Science Foundation of China(12222508)

National Natural Science Foundation of China(U1932213)

National Natural Science Foundation of China(22308346)

Fundamental Research Funds for the Central Universities(WK2060000016)

USTC Research Funds of the Double First-Class Initiative(YD2310002005)

USTC Research Funds of the Double First-Class Initiative(YD9990002014)

National Key R&D Program of China(2023YFA1506304)

Youth Innovation Promotion Association CAS(2020454)

Xiaomi Young Talents Program,Joint Funds from the Hefei National Synchrotron Radiation Laboratory(KY9990000202)

Natural Science Foundation of Anhui Province(2208085QB42)

Instruments Center for Physical Science,University of Science and Technology of China()

出版年

2024

科学通报(英文版)

中国科学院

科学通报(英文版)

CSTPCD

ISSN：1001-6538

参考文献量50

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