Balancing dynamic evolution of active sites for urea oxidation in practical scenarios

Jichao Zhang; Jiexin Zhu; Liqun Kang; Qing Zhang; Longxiang Liu; Fei Guo; Kaiqi Li; Jianrui Feng; Lixue Xia; Lei Lv; Wei Zong; Paul R. Shearing; Dan J. L. Brett; Ivan P. Parkin; Xuedan Song; Liqiang Mai; Guanjie He

doi:10.1039/D3EE03258B

Balancing dynamic evolution of active sites for urea oxidation in practical scenarios†

Jichao Zhang,‡^a Jiexin Zhu,

‡^ab Liqun Kang,‡^c Qing Zhang,‡^d Longxiang Liu,^a Fei Guo,^a Kaiqi Li,^a Jianrui Feng,^a Lixue Xia,^e Lei Lv,^b Wei Zong,

^a Paul R. Shearing,

^f Dan J. L. Brett,

^f Ivan P. Parkin,

*^a Xuedan Song,

*^d Liqiang Mai*^b and Guanjie He

*^af

Author affiliations

* Corresponding authors

^a Christopher Ingold Laboratory, Department of Chemistry, University College London (UCL), 20 Gordon Street, London WC1H 0AJ, UK
E-mail: g.he@ucl.ac.uk, i.p.parkin@ucl.ac.uk

^b State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan Hubei 430070, China
E-mail: mlq518@whut.edu.cn

^c Department of Inorganic Spectroscopy, Max-Planck-Institute for Chemical Energy Conversion, Stiftstr. 34-36, 45470 Mülheim an der Ruhr, Germany

^d School of Chemistry, State Key Lab of Fine Chemicals, Liaoning Key Lab for Energy Materials and Chemical Engineering, Dalian University of Technology, Dalian, Liaoning 116024, China
E-mail: song@dlut.edu.cn

^e State Key Laboratory of Silicate Materials for Architectures, International School of Materials Science and Engineering, Wuhan University of Technology, No. 122 Luoshi Road, Wuhan 430070, China

^f Electrochemical Innovation Lab (EIL), Department of Chemical Engineering, University College London (UCL), London WC1E 7JE, UK

Abstract

Electrochemical urea splitting provides a sustainable and environmentally benign route for facilitating energy conversion. Nonetheless, the sustained efficiency of urea splitting is impeded by a scarcity of active sites during extended operational periods. Herein, an atomic heterostructure engineering strategy is proposed to promote the generation of active species via synthesizing unique Ru–O₄ coordinated single atom catalysts anchored on Ni hydroxide (Ru₁–Ni(OH)₂), with ultralow Ru loading mass of 40.6 μg cm⁻² on the nickel foam for commercial feasibility. Leveraging in situ spectroscopic characterizations, the structure-performance relationship in low and high urea concentrations was investigated and exhibited extensive universality. The boosted generation of dynamic Ni³⁺ active sites ensures outstanding activity and prominent long-term durability tests in various practical scenarios, including 100 h Zn–urea–air battery operation, 100 h alkaline urine electrolysis, and over 400 h stable hydrogen production in membrane electrode assembly (MEA) system under industrial-level current density.

This article is part of the themed collection: Recent Open Access Articles

Energy & Environmental Science

Balancing dynamic evolution of active sites for urea oxidation in practical scenarios†

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