<i>In silico</i> design of dual-doped nitrogenated graphene (C<sub>2</sub>N) employed in electrocatalytic reduction of carbon monoxide to ethylene

Wang, Honglei; Ren, Guoqing; Zhao, Yanliang; Sun, Lanju; Jun, Sun Hee; Yang, Li; Yu, Tie; Deng, Weiqiao; Sun, Lei

doi:10.1039/d1ta09847k

Cited by 17 publications

(7 citation statements)

References 65 publications

(79 reference statements)

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“…The potential of B, P doped C 2 N monolayer as metal-free catalyst for reducing CO to C 2 H 4 was explored (Wang et al, 2022). It was shown that B&P/C 2 N catalysts contribute to C-C coupling and prevent catalyst poisoning due to suitable adsorption energy for CO and lower ethylene desorption energy.…”

Section: Heteronuclear Dacsmentioning

confidence: 99%

“…After the introduction of SeSA, the free energy of CO* decreased from 1.28 (MoSA) to 1.15 eV (MoSA-SeSA), indicating that the synergistic effect of MoSA-SeSA can significantly promote the generation of CO ( Sun et al, 2022 ). The potential of B, P doped C 2 N monolayer as metal-free catalyst for reducing CO to C 2 H 4 was explored ( Wang et al, 2022 ). It was shown that B&P/C 2 N catalysts contribute to C-C coupling and prevent catalyst poisoning due to suitable adsorption energy for CO and lower ethylene desorption energy.…”

Section: Dacsmentioning

confidence: 99%

“…Reproduced with permission. (figure used with permission from Wang et al, 2022 ) (E) Geometric configuration of NiN 4 –O/C and NiN 4 /C in an aqueous solution. Grey, C; blue, N; light blue, Ni; red, O; white, H; yellow, hydronium.…”

Section: Electrode Potential and Solvent Effect On Electrocatalytic C...mentioning

confidence: 99%

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Recent advances in the theoretical studies on the electrocatalytic CO2 reduction based on single and double atoms

Meng

Huang²,

Zhang³

et al. 2023

Front. Chem.

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Excess of carbon dioxide (CO2) in the atmosphere poses a significant threat to the global climate. Therefore, the electrocatalytic carbon dioxide reduction reaction (CO2RR) is important to reduce the burden on the environment and provide possibilities for developing new energy sources. However, highly active and selective catalysts are needed to effectively catalyze product synthesis with high adhesion value. Single-atom catalysts (SACs) and double-atom catalysts (DACs) have attracted much attention in the field of electrocatalysis due to their high activity, strong selectivity, and high atomic utilization. This review summarized the research progress of electrocatalytic CO2RR related to different types of SACs and DACs. The emphasis was laid on the catalytic reaction mechanism of SACs and DACs using the theoretical calculation method. Furthermore, the influences of solvation and electrode potential were studied to simulate the real electrochemical environment to bridge the gap between experiments and computations. Finally, the current challenges and future development prospects were summarized and prospected for CO2RR to lay the foundation for the theoretical research of SACs and DACs in other aspects.

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Section: Heteronuclear Dacsmentioning

confidence: 99%

Section: Dacsmentioning

confidence: 99%

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Recent advances in the theoretical studies on the electrocatalytic CO2 reduction based on single and double atoms

Meng

Huang²,

Zhang³

et al. 2023

Front. Chem.

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“…Besides g‐C 3 N 4 , the nitrogen‐rich 2D carbon nitride family contains several materials, and some of them, including C 2 N, C 3 N, etc., were also studied for electrocatalytic applications in recent years. [ 148–157 ] Taking C 2 N as an example, it consists of benzene rings connected by nitrogen atoms to constitute large six‐membered aromatic rings with two nitrogen atoms facing each other, leading to the formation of periodically uniform 0.83‐nm‐sized holes. [ 155,158 ] Shinde et al.…”

Section: Emerging Graphene Analogues For Efficient Electrocatalysismentioning

confidence: 99%

Emerging Graphene Derivatives and Analogues for Efficient Energy Electrocatalysis

Wang

Tang

Chang-xin

et al. 2022

Adv Funct Materials

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The demand for highly efficient conversion and storage of renewable energy sources calls for advanced electrocatalytic technologies. 2D graphene has long been investigated as a versatile material platform with flexible structure and tunable surface properties for the design of efficient electrocatalysts. In recent years, new types of graphene derivatives and analogues keep emerging and showing great potential for highly active and selective electrocatalytic applications. In this review, recent progresses on emerging graphene derivatives and analogues for electrocatalysis are summarized. This review starts from the introduction of the material requirements for efficient electrocatalysis and the advantages of 2D graphene derivatives and analogues. Then new advances on graphene derivatives for electrocatalysis are introduced, including twisted graphene superlattices, molecular‐level single‐atom catalysts, and graphene‐supported dual‐atom catalysts or atomic clusters. The next section deals with the emerging research directions of graphene analogues for electrocatalysis, including 2D metal‐free materials, metallenes, 2D transition metal borides (MBenes), and new design strategies of them. Finally, an overview on the development status of this field is provided, and perspectives on the future development of efficient electrocatalytic technologies based on 2D materials are proposed.

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“…Many studies have focused on transition-metal surfaces, − metal oxides, , or metal atoms coordinated on substrate surfaces. ,− However, the cost, abundance, and toxicity are always issues for these precious metals. Carbon-based catalysts have an advantage in environmental friendliness, durability, high mobility, and flexible synthesis of different motifs. − The modification of electronic structures is one of the straightforward strategies to improve material properties, and many have utilized B, N, or P atom doping toward sp 2 (graphene) and sp 3 (nanodiamond) carbon atoms for nonmetal catalysis. − However, studies concerning the combination of sp–sp 2 hybrid systems are relatively scarce. Graphyne family members are carbon allotropes consisting of a network of sp 2 and sp hybridization.…”

Section: Introductionmentioning

confidence: 99%

Breaking BEP Relationship with Strong CO Binding and Low C–C Coupling Barriers for Ethanol Synthesis on Boron-Doped Graphyne: Bond Order Conservation and Flexible Orbital Hybridization

Namuangruk

Takahashi

2023

J. Phys. Chem. C

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For CO2 electroreduction to produce C2+ products, many nonmetal catalyst studies have focused on doping to sp2 and sp3 carbon materials for efficient carbon–carbon (CC) bond formation. However, studies on doping to sp hybridization are scarce, so we focused on graphyne (GRY), a stable carbon allotrope with sp–sp2 hybridization. We theoretically showed that ethanol could be selectively produced with a low limiting potential of −0.53 V with a very low CC coupling barrier of 0.46 eV by boron doping (B-GRY) to the highly abundant sp hybrid linker. Fascinatingly, strong CO binding energy coexisted with a low CC coupling barrier, thus breaking the Bell–Evans–Polanyi relation. This provides a new direction that differs from previous studies that utilized the weakening of CO binding energy to reduce the CC coupling barrier. Our calculations using an integrated crystal orbital bond index (ICOBI) showed that for 2*CO, the binding with B-GRY includes both σ donation and π back-donation, while only σ binding with B-GRY occurs for *COCO. The electrons responsible for the π back-donation for CO binding were used for the OC–CO bond formation after CC coupling. The reactive π electron on the sp hybrid linker has a chameleon-like feature changing its orbital hybridization to donate electrons depending on the adsorbate. We utilized the ICOBI along the ethanol production pathway for the first time and showed that the bond order conservation effectively promotes CC coupling on B-GRY.

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In silico design of dual-doped nitrogenated graphene (C₂N) employed in electrocatalytic reduction of carbon monoxide to ethylene

Abstract: The electrocatalytic reduction of carbon monoxide (CO) to valuable multi-carbon chemicals is among the most promising methods to ensure a sustainable carbon cycle. Many catalysts have been developed to achieve...

Cited by 17 publications

References 65 publications

Recent advances in the theoretical studies on the electrocatalytic CO2 reduction based on single and double atoms

Recent advances in the theoretical studies on the electrocatalytic CO2 reduction based on single and double atoms

Emerging Graphene Derivatives and Analogues for Efficient Energy Electrocatalysis

Breaking BEP Relationship with Strong CO Binding and Low C–C Coupling Barriers for Ethanol Synthesis on Boron-Doped Graphyne: Bond Order Conservation and Flexible Orbital Hybridization

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In silico design of dual-doped nitrogenated graphene (C2N) employed in electrocatalytic reduction of carbon monoxide to ethylene

Abstract: The electrocatalytic reduction of carbon monoxide (CO) to valuable multi-carbon chemicals is among the most promising methods to ensure a sustainable carbon cycle. Many catalysts have been developed to achieve...

Cited by 17 publications

References 65 publications

Recent advances in the theoretical studies on the electrocatalytic CO2 reduction based on single and double atoms

Recent advances in the theoretical studies on the electrocatalytic CO2 reduction based on single and double atoms

Emerging Graphene Derivatives and Analogues for Efficient Energy Electrocatalysis

Breaking BEP Relationship with Strong CO Binding and Low C–C Coupling Barriers for Ethanol Synthesis on Boron-Doped Graphyne: Bond Order Conservation and Flexible Orbital Hybridization

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In silico design of dual-doped nitrogenated graphene (C₂N) employed in electrocatalytic reduction of carbon monoxide to ethylene