Ultralow Overpotential of Hydrogen Evolution Reaction using Fe‐Doped Defective Graphene: A Density Functional Study

Lim, Juhyung; Back, Seoin; Choi, Changhyeok; Jung, Yousung

doi:10.1002/cctc.201800635

Cited by 23 publications

(18 citation statements)

References 60 publications

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“… 19 − 21 Among them, the most reported SACs are limited to transition-metal atoms (Fe, Co, Ni, Cu, etc.) supported by heteroatom N-doped carbonaceous materials, which can be applied to the catalysis of a wide range of electrochemical reactions of ORR, 22 − 28 nitrogen reduction reaction (NRR), 29 − 34 carbon dioxide reduction reaction (CO 2 RR), 35 − 41 hydrogen reduction reaction (HER), 42 − 44 OER, 8 , 45 , 46 etc. The single metal atom and its coordination environment are usually modeled by a MN 4 moiety having a metal center coordinated with four N atoms.…”

Section: Introductionmentioning

confidence: 99%

Simultaneously Enhancing Catalytic Performance and Increasing Density of Bifunctional CuN₃ Active Sites in Dopant-Free 2D C₃N₃Cu for Oxygen Reduction/Evolution Reactions

et al. 2022

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Atomically dispersed M–N–C has been considered an effective catalyst for various electrochemical reactions such as oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), which faces the challenge of increasing metal load while simultaneously maintaining catalytic performance. Herein, we put forward a strategy for boosting catalytic performances of a single Cu atom coordinated with three N atoms (CuN 3 ) for both ORR and OER by increasing the density of connected CuN 3 moieties. Our calculations first show that a single CuN 3 moiety exhibiting no catalytic performance for ORR and OER can be activated by increasing the density of metal centers, which weakens the binding affinity to *OH due to the lowered d-band center of the metal atoms. These findings stimulate the further theoretical design of a two-dimensional compound of C 3 N 3 Cu with a high concentration of homogeneously distributed CuN 3 moieties serving as bifunctional active sites, which demonstrates efficient catalytic performance for both ORR and OER as reflected by the overpotentials of 0.71 and 0.43 V, respectively. This work opens a new avenue for designing effective single-atom catalysts with potential applications as energy storage and conversion devices possessing high density of metal centers independent of the doping strategy and defect engineering, which deserves experimental investigation in the future.

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Section: Introductionmentioning

confidence: 99%

Simultaneously Enhancing Catalytic Performance and Increasing Density of Bifunctional CuN₃ Active Sites in Dopant-Free 2D C₃N₃Cu for Oxygen Reduction/Evolution Reactions

et al. 2022

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“…In recent years, non‐precious metal based OER catalysts, such as transition‐metal compounds, carbon‐based materials, and black phosphorus, develop rapidly and have demonstrated advanced performance toward catalyzing OER. Additionally, since the concept of single atom catalysts (SACs) was firstly proposed by Zhang et al., SACs have shown significant advantages in hydrogen evolution reaction (HER), CO oxidation, oxygen reduction reaction (ORR), nitrogen reduction reaction(NRR), as well as OER . Fei et al.…”

Section: Introductionmentioning

confidence: 99%

Cu Anchored Ti₂NO₂ as High Performance Electrocatalyst for Oxygen Evolution Reaction: A Density Functional Theory Study

et al. 2020

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MXenes have attracted great attention in the fields of energy conversion and catalysis, and have proved to be an effective supporting material for single atom catalysts (SACs). In the present study, we investigated the catalytic activity of a series mono‐atomic transition‐metal atoms supported by MXenes M2NO2 for oxygen evolution reaction (OER) via first principle calculation. Particularly, single atom Cu site on Ti2NO2 having the lowest overpotentials of 0.24 V and bonding with the reaction intermediates moderately, is the most active SAC for OER. Energetically, Cu atom prefers to be mono‐atomically anchored on Ti2NO2 instead of aggregating. Plus, Cu anchoring enhance the electronic states around Fermi level. Additionally, ab‐initio molecular dynamics simulations show that Cu atom is anchored on Ti2NO2, stable and isolatable at 300 K. Studies on the small molecule adsorption on Cu‐Ti2NO2 further prove the potential applications of Cu−Ti2NO2 as active SACs for OER. Our results broaden the perception of MXenes and guide the exploration of non‐noble metal based OER electrocatalysts.

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“…The graph shows that the theoretical overpotential is usually higher than that obtained experimentally, whereas the difference is not large. For example, the overpotentials in the simulation versus experiment are −0.03 versus −0.032 V and −0.004 versus −0.066 V for Co–1T MoS 2 [ 51 ] and Fe–C 3 , [ 52 ] respectively, proving that the simulated data predicts the experimental results well. Therefore, we compared the overpotential obtained from the simulations in this study with the theoretical and experimental data of other 2D catalytic materials derived previously.…”

Section: Resultsmentioning

confidence: 68%

“…Therefore, we compared the overpotential obtained from the simulations in this study with the theoretical and experimental data of other 2D catalytic materials derived previously. On the one hand, for different substrate SACs, TMs–Ti 2 CT x (Rh–Ti 2 CT x −0.0026 V) has a lower overpotential than other 2D material‐based SACs (graphene and MoS 2 ), with the lowest overpotential of –0.003 V for Fe–C 3 [ 52a ] and –0.015 V for Os–1T MoS 2 [ 53 ] in simulations. Considering Ir–SACs as an example, the Ti 2 CT x substrate (–0.009 V) showed superior catalytic performance over MoS 2 substrates (–0.044 V), [ 54 ] illustrating the superior performance of MXene substrates for single‐atom loading.…”

Section: Resultsmentioning

confidence: 99%

Single Atom‐Modified Hybrid Transition Metal Carbides as Efficient Hydrogen Evolution Reaction Catalysts

Wei

Legut

et al. 2021

Adv Funct Materials

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2D transition metal carbides and nitrides (MXenes) are promising hydrogen evolution reaction (HER) catalysts owing to their metallic conductivity, abundant surface active sites, and high specific surface area. The introduction of a single transition metal atom (TM) at the surface is a good way to improve the HER performance of MXenes. However, the effect of TM on MXenes in previous theoretical studies focused on pure functional groups, and ignored the hybrid‐functionalized ones, which are mostly observed in experiments. Herein, the HER performance of four O/F ratios stable hybrids MXenes, Ti2CTx (T = O, F), is explored. Ti2CO1.33F0.67 exhibits superior HER catalytic activity, comparable to that of platinum metals. Further combinatorial screening of ≈200 TMs based on Ti2CTx structures suggests that Rh, Ti, Ir, and Pt are optimal TM candidates that enhance the sensitivity to strain modulation and reduce the activation barrier for hydrogen generation. A descriptor ψ is used to quantify HER performance and reveals the role of the electron filling of TM to the antibonding orbitals. These findings propose feasible candidates with high HER performance through single‐atom modification for hybrid‐functional MXenes, and a useful descriptor to screen for MXenes with desirable catalytic properties.

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Ultralow Overpotential of Hydrogen Evolution Reaction using Fe‐Doped Defective Graphene: A Density Functional Study

Cited by 23 publications

References 60 publications

Simultaneously Enhancing Catalytic Performance and Increasing Density of Bifunctional CuN₃ Active Sites in Dopant-Free 2D C₃N₃Cu for Oxygen Reduction/Evolution Reactions

Simultaneously Enhancing Catalytic Performance and Increasing Density of Bifunctional CuN₃ Active Sites in Dopant-Free 2D C₃N₃Cu for Oxygen Reduction/Evolution Reactions

Cu Anchored Ti₂NO₂ as High Performance Electrocatalyst for Oxygen Evolution Reaction: A Density Functional Theory Study

Single Atom‐Modified Hybrid Transition Metal Carbides as Efficient Hydrogen Evolution Reaction Catalysts

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Ultralow Overpotential of Hydrogen Evolution Reaction using Fe‐Doped Defective Graphene: A Density Functional Study

Cited by 23 publications

References 60 publications

Simultaneously Enhancing Catalytic Performance and Increasing Density of Bifunctional CuN3 Active Sites in Dopant-Free 2D C3N3Cu for Oxygen Reduction/Evolution Reactions

Simultaneously Enhancing Catalytic Performance and Increasing Density of Bifunctional CuN3 Active Sites in Dopant-Free 2D C3N3Cu for Oxygen Reduction/Evolution Reactions

Cu Anchored Ti2NO2 as High Performance Electrocatalyst for Oxygen Evolution Reaction: A Density Functional Theory Study

Single Atom‐Modified Hybrid Transition Metal Carbides as Efficient Hydrogen Evolution Reaction Catalysts

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Simultaneously Enhancing Catalytic Performance and Increasing Density of Bifunctional CuN₃ Active Sites in Dopant-Free 2D C₃N₃Cu for Oxygen Reduction/Evolution Reactions

Simultaneously Enhancing Catalytic Performance and Increasing Density of Bifunctional CuN₃ Active Sites in Dopant-Free 2D C₃N₃Cu for Oxygen Reduction/Evolution Reactions

Cu Anchored Ti₂NO₂ as High Performance Electrocatalyst for Oxygen Evolution Reaction: A Density Functional Theory Study