Pd doping-weakened intermediate adsorption to promote electrocatalytic nitrate reduction on TiO2 nanoarrays for ammonia production and energy supply with zinc-nitrate batteries

Research output: Journal Publications and Reviews (RGC: 21, 22, 62)21_Publication in refereed journalpeer-review

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Detail(s)

Original languageEnglish
Pages (from-to)3938-3944
Journal / PublicationEnergy & Environmental Science
Volume14
Issue number7
Online published14 Jun 2021
Publication statusPublished - 1 Jul 2021

Abstract

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 N≡N 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 N=O 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.

Research Area(s)

  • NITROGEN, CATALYSTS, STORAGE

Citation Format(s)