Designing C3N-supported single atom catalysts for efficient nitrogen reduction based on descriptor of catalytic activity

Nong, Wei; Qin, Shihan; Huang, Fan; Liang, Haikuan; Yang, Zhen; Qi, Chenze; Yan, Lifeng; Wang, Chengxin

doi:10.1016/j.carbon.2021.05.066

Cited by 32 publications

(25 citation statements)

References 73 publications

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“…In the last 3–4 years, several contributions appeared in the literature where correlations or descriptors have been proposed for electrocatalytic reactions such as the oxygen reduction (ORR), the oxygen evolution (OER), and the hydrogen evolution (HER) reactions, or N 2 and CO 2 reduction. − Sometimes these descriptors correspond to a specific physical property of a SAC, such as the electronegativity of the transition metal center, number of d electrons, position of the d states with respect to the vacuum level, computed charge of the metal atom, electronegativity of neighboring atoms, energy position of bonding or antibonding combinations, etc. However, a simple direct correlation with just one of these variables for a representative number of cases is missing.…”

Section: Introductionmentioning

confidence: 99%

Universal Principles for the Rational Design of Single Atom Electrocatalysts? Handle with Care

2022

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One of the objectives of electronic structure theory is to predict chemical and catalytic activities. This is a challenging target due to the large number of variables that determine the performance of a heterogeneous catalyst. The complexity of the problem has reduced considerably with the advent of single atom catalysts (SACs) and, in particular, of graphene-based SACs for electrocatalytic reactions such as the oxygen reduction (ORR), the oxygen evolution (OER), and the hydrogen evolution (HER) reactions. In this context we assist with a rapidly growing number of theoretical studies based on density functional theory (DFT) and with proposals of universal descriptors that should provide a guide to the experimentalist for the synthesis of efficient catalysts. In this Perspective we critically analyze some of the current problems connected with the prediction of the activity of SACs: accuracy of the calculations, neglect of important contributions in the models used, physical meaning of the proposed descriptors, not to mention some problems of reproducibility. It follows that the “rational design” of a catalyst based on some of the proposed universal descriptors should be considered with caution.

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Section: Introductionmentioning

confidence: 99%

Universal Principles for the Rational Design of Single Atom Electrocatalysts? Handle with Care

2022

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“…We note that there are previous reports where DG NNH* has been used as a descriptor to screen the eNRR performance of various catalysts. 12,46,59,64,73,76 We nd that O val , the valence electron occupancy of the metal center, is an electronic descriptor which exhibits a volcano-type relationship with h NRR for all 66 SACs (see Fig. 3b).…”

Section: Resultsmentioning

confidence: 94%

“…This underlines the key role played by the NNH* step in eNRR and confirms that ΔG NNH * is an energy descriptor for the performance of SACs toward eNRR. We note that there are previous reports where ΔG NNH * has been used as a descriptor to screen the eNRR performance of various catalysts 12,46,59,64,73,76 . We find that O val , the valence electron occupancy of the metal center, is an electronic descriptor which exhibits a volcano-type relationship with η NRR for all 66 SACs (see…”

Section: Resultsmentioning

confidence: 96%

“…V respectively 62 Earlier authors have proposed various descriptors to capture the behavior of catalysts [67][68][69][70][71][72][73][74][75][76][77][78][79][80] .…”

Section: Resultsmentioning

confidence: 99%

“…Earlier authors have proposed various descriptors to capture the behavior of catalysts. [67][68][69][70][71][72][73][74][75][76][77][78][79][80] We demonstrate two such descriptors: an energetic one and an electronic one, to correlate with h NRR for the SACs considered here. On plotting the data for all 66 systems, we see (Fig.…”

Section: Resultsmentioning

confidence: 99%

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Descriptors and graphical construction forin silicodesign of efficient and selective single atom catalysts for the eNRR

2022

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A DFT Investigation of B‐Doped C₃N as Single Atom Electrocatalysts for N₂‐to‐NH₃ Conversion

Ma,

Du,

Song

et al. 2023

ChemPhysChem

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The NH3 synthesis from N2 plays an important role in the ecological cycle and industrial production. Different from industrial NH3 synthesis with high pollution and energy consumption, electrocatalytic NH3 synthesis is favored because of its environmental protection, energy saving, ambient reaction conditions and other characteristics. However, due to the low efficiency and poor reaction selectivity of the existing electrocatalysts, which can not be used actually, the development of new electrocatalysts for nitrogen reduction reaction (NRR) is particularly urgent. Herein, we designed a series of transition metal atoms anchored B‐doped defective C3N surface (TM@B2C3N) as single‐atom catalysts. Through the screening process of N2 adsorption activation, N2H formation and NH3 desorption, finally the excellent electrocatalysts with strong stability and high activity (Cr@B2C3N and Mn@B2C3N) were obtained. After simulating the entire pathway, it was found that the NRR process on Cr@B2C3N and Mn@B2C3N via consecutive and distal pathways with the lowest limiting potential of −0.42 and −0.52 V, which have the good ability to inhibit hydrogen evolution reaction. Finally, the electronic properties were analyzed, and the reason for their high catalytic activity was summarized. This work provides a new idea for the rational design of NRR electrocatalysts and promotes the practical application of electrocatalysts.

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Designing C3N-supported single atom catalysts for efficient nitrogen reduction based on descriptor of catalytic activity

Cited by 32 publications

References 73 publications

Universal Principles for the Rational Design of Single Atom Electrocatalysts? Handle with Care

Universal Principles for the Rational Design of Single Atom Electrocatalysts? Handle with Care

Descriptors and graphical construction forin silicodesign of efficient and selective single atom catalysts for the eNRR

A DFT Investigation of B‐Doped C₃N as Single Atom Electrocatalysts for N₂‐to‐NH₃ Conversion

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Designing C3N-supported single atom catalysts for efficient nitrogen reduction based on descriptor of catalytic activity

Cited by 32 publications

References 73 publications

Universal Principles for the Rational Design of Single Atom Electrocatalysts? Handle with Care

Universal Principles for the Rational Design of Single Atom Electrocatalysts? Handle with Care

Descriptors and graphical construction forin silicodesign of efficient and selective single atom catalysts for the eNRR

A DFT Investigation of B‐Doped C3N as Single Atom Electrocatalysts for N2‐to‐NH3 Conversion

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A DFT Investigation of B‐Doped C₃N as Single Atom Electrocatalysts for N₂‐to‐NH₃ Conversion