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DOI10.1039/d1ee00806d
Pd doping-weakened intermediate adsorption to promote electrocatalytic nitrate reduction on TiO2nanoarrays for ammonia production and energy supply with zinc-nitrate batteries
Guo Y.; Zhang R.; Zhang S.; Zhao Y.; Yang Q.; Huang Z.; Dong B.; Zhi C.
发表日期2021
ISSN17545692
起始页码3938
结束页码3944
卷号14期号:7
英文摘要The (photo)electrochemical nitrogen reduction reaction for ammonia (NH3) production is an appealing alternative to the traditional high-energy Haber-Bosch reaction. However, the future of this approach is bleak because of the ultralow N2 solubility and the nonpolar NN bond causing the NH3 yield and selectivity to be unsatisfactory. Nitrate electroreduction (NORR) into NH3 brings promise for the future landscape of NH3 electrosynthesis due to the low NO bond energy and high nitrate solubility. Here, we report a highly efficient Pd-doped TiO2 nanoarray electrode for NH3 production from the NORR. With weakened adsorption abilities to the intermediates induced by Pd introduction, the catalyst delivers a record-high NH3 yield of 1.12 mg cm-2 h-1 (or 0.066 mmol cm-2 h-1), an impressive NH3 faradaic efficiency (FE) of 92.1%, and an exceptional nitrate conversion of 99.6%. Considering an eight-electron nitrate-to-ammonia reaction and the excellent electrocatalytic activity of Pd/TiO2, we, for the first time, propose and develop a Zn-nitrate battery system, which delivers striking bifunctionality for harnessing the electrons related to the NORR to generate electricity and directly produce NH3, specified by a power density of 0.87 mW cm-2 and a high NH3 FE of 81.3%. Our work not only verifies the positive effect of Pd doping on facilitating the NORR, but also demonstrates a galvanic nitrate-based cell providing a promising strategy for NH3 production and broadening the field of Zn-based batteries. © The Royal Society of Chemistry.
英文关键词Ammonia; Electric batteries; Electric power generation; Electrolytic reduction; Nitrates; Oxide minerals; Palladium; Solubility; Titanium dioxide; Adsorption ability; Ammonia production; Electro reduction; Electrocatalytic activity; Electrocatalytic nitrate reduction; Faradaic efficiencies; Generate electricity; Nitrogen reduction; Zinc compounds; adsorption; ammonia; array; catalysis; electricity supply; electrokinesis; fuel cell; nanoparticle; nitrate; palladium; reduction
语种英语
来源期刊Energy & Environmental Science
文献类型期刊论文
条目标识符http://gcip.llas.ac.cn/handle/2XKMVOVA/190614
作者单位Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, 999077, Hong Kong; National Engineering Research Center for Advanced Polymer Processing Technology, Zhengzhou University, Henan, Zhengzhou, 450002, China; Centre for Functional Photonics, City University of Hong Kong, Kowloon, Hong Kong
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GB/T 7714
Guo Y.,Zhang R.,Zhang S.,et al. Pd doping-weakened intermediate adsorption to promote electrocatalytic nitrate reduction on TiO2nanoarrays for ammonia production and energy supply with zinc-nitrate batteries[J],2021,14(7).
APA Guo Y..,Zhang R..,Zhang S..,Zhao Y..,Yang Q..,...&Zhi C..(2021).Pd doping-weakened intermediate adsorption to promote electrocatalytic nitrate reduction on TiO2nanoarrays for ammonia production and energy supply with zinc-nitrate batteries.Energy & Environmental Science,14(7).
MLA Guo Y.,et al."Pd doping-weakened intermediate adsorption to promote electrocatalytic nitrate reduction on TiO2nanoarrays for ammonia production and energy supply with zinc-nitrate batteries".Energy & Environmental Science 14.7(2021).
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