Tuning the Coordination Structure of Cu-N-C Single Atom Catalysts for Simultaneous Electrochemical Reduction of CO_2 and NO_3~ – to Urea

Josh Leverett; Thanh Tran-Phu; Jodie A. YuwonoPriyank KumarChangmin KimQingfeng ZhaiChen HanJiangtao QuJulie CairneyAlexandr N. SimonovRosalie K. HockingLiming DaiRahman DaiyanRose Amal

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Tuning the Coordination Structure of Cu-N-C Single Atom Catalysts for Simultaneous Electrochemical Reduction of CO_2 and NO_3~ – to Urea

机译：Tuning the Coordination Structure of Cu-N-C Single Atom Catalysts for Simultaneous Electrochemical Reduction of CO_2 and NO_3~ – to Urea

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Closing both the carbon and nitrogen loops is a critical venture to supportthe establishment of the circular, net-zero carbon economy. Althoughsingle atom catalysts (SACs) have gained interest for the electrochemicalreduction reactions of both carbon dioxide (CO_2RR) and nitrate (NO_3RR),the structure–activity relationship for Cu SAC coordination for these reactionsremains unclear and should be explored such that a fundamentalunderstanding is developed. To this end, the role of the Cu coordinationstructure is investigated in dictating the activity and selectivity for the CO_2RRand NO_3RR. In agreement with the density functional theory calculations,it is revealed that Cu-N_4 sites exhibit higher intrinsic activity toward theCO2RR, whilst both Cu-N_4 and Cu-N_(4?x)-C_x sites are active toward the NO3RR.Leveraging these findings, CO2RR and NO3RR are coupled for the formationof urea on Cu SACs, revealing the importance of *COOH binding as acritical parameter determining the catalytic activity for urea production. Tothe best of the authors’ knowledge, this is the first report employing SACsfor electrochemical urea synthesis from CO_2RR and NO_3RR, which achievesa Faradaic efficiency of 28% for urea production with a current density of?27 mA cm~(–2) at ?0.9 V versus the reversible hydrogen electrode.

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《Advanced energy materials》 |2022年第32期|2201500.1-2201500.9|共9页
作者
Josh Leverett; Thanh Tran-Phu; Jodie A. YuwonoPriyank KumarChangmin KimQingfeng ZhaiChen HanJiangtao QuJulie CairneyAlexandr N. SimonovRosalie K. HockingLiming DaiRahman DaiyanRose Amal;
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Australian Centre for Microscopy and MicroanalysisThe University of SydneySydney, New South Wales 2006, Australia;

School of Chemistry and the ARC Centre of Excellence forElectromaterials ScienceMonash UniversityMelbourne, VIC 3800, Australia;

School of ScienceSwinburne University of TechnologyMelbourne, VIC 3122, AustraliaSchool of Chemical EngineeringUNSW SydneySydney, NSW 2052, AustraliaResearch School of ChemistryThe Australian National UniversityCanberra, ACT 2601, AustraliaSchool of Chemical EngineeringUNSW SydneySydney, NSW 2052, Australia,College of Engineering and Computer ScienceAustralian National UniversityCanberra, ACT 2601, Australia;

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CO_2 reduction; Cu single atom; power to X; urea;

Tuning the Coordination Structure of Cu-N-C Single Atom Catalysts for Simultaneous Electrochemical Reduction of CO_2 and NO_3~ – to Urea

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