Amorphous iron-doped nickel boride with facilitated structural reconstruction and dual active sites for efficient urea electrooxidation

Chen，Zhijie1,2; Zheng，Renji3; Zou，Haiyuan4; Wang，Ranhao1; Huang，Changzhu1; Dai，Wei1; Wei，Wei2; Duan，Lele4; Ni，Bing Jie2; Chen，Hong1

2023-06-01

10.1016/j.cej.2023.142684

Chemical Engineering Journal   影响因子和分区

1385-8947

1873-3212

Designing transition metal-based catalysts for efficient urea oxidation reaction (UOR) is important for realizing energy-saving hydrogen production via urea-rich (waste)water electrolysis. Herein, we have developed an iron-doped amorphous nickel boride electrocatalyst (aFe-NiB) for UOR. Compared with the undoped and crystalline counterparts, aFe-NiB exhibits a higher activity and the benchmark current density of 10 mA cm can be attained at 1.298 V vs. reversible hydrogen electrode (RHE). Coupled with an efficient hydrogen evolution catalyst, the aFe-NiB-assisted urine electrolyzer can attain a 46 times higher H production rate than the water electrolyzer at 1.50 V. Further study reveals a crystallinity-dependent structure self-reconstruction process during UOR. aFe-NiB attains complete phase evolution from boride to electroactive Fe-doped NiOOH. In addition, density functional theory calculations imply that Fe dopants can improve intrinsic catalytic activity via electronic structure regulation of the self-evolved NiOOH and forming heterogeneous bimetallic active sites for UOR. This study provides meaningful insights into the crystallinity-dependent UOR performance and effective strategies to develop efficient UOR (pre)catalysts with dual active sites. Significantly, the demonstrated direct wastewater (urine) electrolysis paves the way for net zero buildings -targeted human waste reutilization.

Amorphous electrocatalysts Borides Hydrogen energy Structural reconstruction Urine electrolysis

SCI ; EI

英语

ESI高被引

第一

National Key Research and Development Program of China[2021YFA1202500] ; National Natural Science Foundation of China[61875119] ; Foundation of Shenzhen Science, Technology and Innovation Commission (SSTIC)[JCYJ20200109141625078] ; Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials[ZDSYS20200421111401738] ; Natural Science Funds for Distinguished Young Scholar of Guangdong Province, China[2020B151502094] ; Australian Research Council (ARC)[DP220101139]

Engineering

Engineering, Environmental ; Engineering, Chemical

WOS:000980678500001

ELSEVIER SCIENCE SA

20231613901379

Borides ; Catalyst activity ; Crystallinity ; Density functional theory ; Electrolysis ; Electronic structure ; Electrooxidation ; Energy conservation ; Hydrogen production ; Iron ; Metabolism ; Nickel ; Nickel compounds ; Urea

Gas Fuels:522 ; Energy Conservation:525.2 ; Iron:545.1 ; Nickel:548.1 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2 ; Ceramics:812.1 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4 ; Crystalline Solids:933.1

ENGINEERING

2-s2.0-85152708614

Scopus

1.State Environmental Protection Key Laboratory of Integrated Surface Water-Groundwater Pollution Control,Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials (SKLISEM),School of Environmental Science and Engineering,Southern University of Science and Technology,Shenzhen,518055,China
2.Centre for Technology in Water and Wastewater,School of Civil and Environmental Engineering,University of Technology Sydney,2007,Australia
3.School of Minerals Processing and Bioengineering,Central South University,Changsha,410083,China
4.Department of Chemistry and Shenzhen Grubbs Institute,Southern University of Science and Technology,Shenzhen,518055,China

Chen，Zhijie,Zheng，Renji,Zou，Haiyuan,et al. Amorphous iron-doped nickel boride with facilitated structural reconstruction and dual active sites for efficient urea electrooxidation[J]. Chemical Engineering Journal,2023,465.

Chen，Zhijie.,Zheng，Renji.,Zou，Haiyuan.,Wang，Ranhao.,Huang，Changzhu.,...&Chen，Hong.(2023).Amorphous iron-doped nickel boride with facilitated structural reconstruction and dual active sites for efficient urea electrooxidation.Chemical Engineering Journal,465.

Chen，Zhijie,et al."Amorphous iron-doped nickel boride with facilitated structural reconstruction and dual active sites for efficient urea electrooxidation".Chemical Engineering Journal 465(2023).