Tuning the Coordination Structure of CuNC Single Atom Catalysts for Simultaneous Electrochemical Reduction of CO2 and NO3– to Urea

Leverett, Joshua; Trần‐Phú, Thành; Yuwono, Jodie A.; Kumar, Priyank V.; Kim, Changmin; Zhai, Qingfeng; Han, Chen; Qu, Jiangtao; Cairney, Julie M.; Simonov, Alexandr N.; Hocking, Rosalie K.; Dai, Liming; Daiyan, Rahman; Amal, Rose

doi:10.1002/aenm.202201500

Cited by 163 publications

(127 citation statements)

References 51 publications

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“…Wang et al explored oxygen vacancy-enriched CeO 2 for urea synthesis from NO 3 – /CO 2 simultaneous reduction, on which the oxygen vacancy could stabilize the intermediate species . Amal and co-workers first reported Cu–N–C single atom catalysts for simultaneous electrochemical reduction of CO 2 and NO 3 – to urea, which achieved 28% FE (urea) with a current density of −27 mA cm –2 at −0.9 V . Other valuable products such as alkylamines were also expanded from electrochemical coreduction of CO 2 and NO 3 – .…”

Section: Basic Experimental Details For Urea Electrosynthesismentioning

confidence: 99%

“…45 Wang et al explored oxygen vacancy-enriched CeO 2 for urea synthesis from NO 3 − /CO 2 simultaneous reduction, on which the oxygen vacancy could stabilize the intermediate species. 35 Amal and coworkers first reported Cu−N−C single atom catalysts for simultaneous electrochemical reduction of CO 2 and NO 3 − to urea, which achieved 28% FE (urea) with a current density of −27 mA cm −2 at −0.9 V. 46 Other valuable products such as alkylamines were also expanded from electrochemical coreduc-tion of CO 2 and NO 3 − . For example, Wang et al first synthesized methylamine (CH 3 NH 2 ) using CoPc-NH 2 /CNT as the catalyst with 13% FE(CH 3 NH 2 ) at −0.92 V. 47 Meanwhile, the same team reported the first electrochemical conversion of CO 2 and NO 3…”

Section: ■ Introductionmentioning

confidence: 99%

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Recent Progress in Electrocatalytic Urea Synthesis under Ambient Conditions

Mei

Zhou

et al. 2022

ACS Sustainable Chem. Eng.

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Industrial urea synthesis is performed under harsh conditions requiring huge energy consumption and accompanied by heavy environmental pollution. Electrocatalytic C− N coupling for valuable urea synthesis from the coreduction of CO 2 and an inexpensive nitrogen source, such as N 2 , nitrite, nitrate, and NO, under ambient conditions is a potential green and sustainable substitute for the harsh industrial process. However, the nuts and bolts of electrocatalytic urea synthesis are seldom systemically reviewed. In this Perspective, theoretical and experimental research progress toward urea electrosynthesis is introduced and critically highlighted. From the view of the reaction pathway for the generation of urea molecules, chemiadsorption and activation of inert molecules (CO 2 or N 2 ) and the subsequent C−N couplings are the most important steps to determine the efficiency and selectivity of electrocatalytic reactions. The mechanisms of C−N coupling and hydrogenation toward urea formation in the above progress are summarized and rigorously estimated. This perspective reviews the exploration and preparation of electrocatalysts for urea synthesis with high efficiency and selectivity.

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Section: Basic Experimental Details For Urea Electrosynthesismentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Recent Progress in Electrocatalytic Urea Synthesis under Ambient Conditions

Mei

Zhou

et al. 2022

ACS Sustainable Chem. Eng.

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“…More significantly, the industrial urea synthesis approach (2NH 3 + CO 2 → CO(NH 2 ) 2 + H 2 O) is still operated under harsh conditions, which leads to complexity and inefficiency for the overall process . The direct urea electrosynthesis approach can be driven with electricity, nitrogen-containing feedstocks, carbon oxides, and water under ambient conditions, ,− which is highly sustainable. Chemists have been seeking catalysts that enable selective C–N coupling to pursue high-efficiency electrocatalytic urea production.…”

Section: P-block-element-based Electrocatalysts For Urea Synthesismentioning

confidence: 99%

“…However, most TM-based electrocatalysts have exhibited low selectivity and FE because they favor side reactions that generate many byproducts (NH 3 , H 2 , CO, etc.) during the electrocatalysis process. ,, Intrigued by the achievements in N 2 /NO 3 – reduction reactions with p-block-element-based electrocatalysts, research efforts have been devoted to exploring such materials for electrochemical C–N coupling.…”

Section: P-block-element-based Electrocatalysts For Urea Synthesismentioning

confidence: 99%

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Emerging p-Block-Element-Based Electrocatalysts for Sustainable Nitrogen Conversion

Liu

Lee

et al. 2022

ACS Nano

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Artificial nitrogen conversion reactions, such as the production of ammonia via dinitrogen or nitrate reduction and the synthesis of organonitrogen compounds via C−N coupling, play a pivotal role in the modern life. As alternatives to the traditional industrial processes that are energy-and carbon-emission-intensive, electrocatalytic nitrogen conversion reactions under mild conditions have attracted significant research interests. However, the electrosynthesis process still suffers from low product yield and Faradaic efficiency, which highlight the importance of developing efficient catalysts. In contrast to the transition-metal-based catalysts that have been widely studied, the p-block-element-based catalysts have recently shown promising performance because of their intriguing physiochemical properties and intrinsically poor hydrogen adsorption ability. In this Perspective, we summarize the latest breakthroughs in the development of p-block-elementbased electrocatalysts toward nitrogen conversion applications, including ammonia electrosynthesis from N 2 reduction and nitrate reduction and urea electrosynthesis using nitrogen-containing feedstocks and carbon dioxide. The catalyst design strategies and the underlying reaction mechanisms are discussed. Finally, major challenges and opportunities in future research directions are also proposed.

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High‐Throughput Screening of Heterogeneous Transition Metal Dual‐Atom Catalysts by Synergistic Effect for Nitrate Reduction to Ammonia

Shu¹,

Chen²,

Liu³

et al. 2023

Adv Funct Materials

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Nitrate reduction to ammonia has attracted much attention for nitrate (NO3‐) removal and ammonia (NH3) production. Identifying promising catalyst for active nitrate electroreduction reaction (NO3RR) is critical to realize efficient upscaling synthesis of NH3 under low‐temperature condition. For this purpose, by means of spin‐polarized first‐principles calculations, the NO3RR performance on a series of graphitic carbon nitride (g‐CN) supported double‐atom catalysts (denoted as M1M2@g‐CN) are systematically investigated. The synergistic effect of heterogeneous dual‐metal sites can bring out tunable activity and selectivity for NO3RR. Amongst 21 candidates examined, FeMo@g‐CN and CrMo@g‐CN possess a high performance with low limiting potentials of ‐0.34 and ‐0.39 V, respectively. The activities can be attributed to a synergistic effect of the M1M2 dimer d orbitals coupling with the anti‐bonding orbital of NO3‐. The dissociation of deposited FeMo and CrMo dimers into two separated monomers is proved to be difficult, ensuring the kinetic stability of M1M2@g‐CN. Furthermore, the dual‐metal decorated on g‐CN significantly reduces the bandgap of g‐CN and broadens the adsorption window of visible light, implying its great promise for photocatalysis. This work opens a new avenue for future theoretical and experimental design related to NO3RR photo‐/electrocatalysts.

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Tuning the Coordination Structure of CuNC Single Atom Catalysts for Simultaneous Electrochemical Reduction of CO₂ and NO₃^– to Urea

Cited by 163 publications

References 51 publications

Recent Progress in Electrocatalytic Urea Synthesis under Ambient Conditions

Recent Progress in Electrocatalytic Urea Synthesis under Ambient Conditions

Emerging p-Block-Element-Based Electrocatalysts for Sustainable Nitrogen Conversion

High‐Throughput Screening of Heterogeneous Transition Metal Dual‐Atom Catalysts by Synergistic Effect for Nitrate Reduction to Ammonia

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