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

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

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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.

Nitrate reductionAlkali cationsPotassiumNi single-atom catalystAmmonia

Yida Zhang、Zhentao Ma、Shaokang Yang、Qingyu Wang、Limin Liu、Yu Bai、Dewei Rao、Gongming Wang、Hongliang Li、Xusheng Zheng

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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

School of Materials Science and Engineering,Jiangsu University,Zhenjiang 212013,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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National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaFundamental Research Funds for the Central UniversitiesUSTC Research Funds of the Double First-Class InitiativeUSTC Research Funds of the Double First-Class InitiativeNational Key R&D Program of ChinaYouth Innovation Promotion Association CASXiaomi Young Talents Program,Joint Funds from the Hefei National Synchrotron Radiation LaboratoryNatural Science Foundation of Anhui ProvinceInstruments Center for Physical Science,University of Science and Technology of China

12222508U193221322308346WK2060000016YD2310002005YD99900020142023YFA15063042020454KY99900002022208085QB42

2024

10.1016/j.scib.2024.02.011

科学通报(英文版)
中国科学院

科学通报(英文版)

CSTPCD
ISSN：1001-6538
年,卷(期)：2024.69(8)
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