Theoretical exploration of the nitrogen fixation mechanism of two-dimensional dual-metal TM1TM2@C9N4 electrocatalysts

Sun, Jinxin; Peng, Xia; Lin, Yuxing; Zhang, Yunfan; Chen, Anjie; Shi, Li; Liu, Yongjun; Niu, Xianghong; He, Ai‐Lei; Zhang, Xiuyun

doi:10.1039/d2nh00451h

Cited by 12 publications

(2 citation statements)

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“…In recent years, single-atom catalysts (SACs) fabricated via doping or adsorbing single transition metal (TM) atoms on suitable substrates have become attractive alternatives and offer unique advantages such as high atom utilization and high catalytic activity derived from abundant active centers with unsaturated coordination. [8][9][10] Even though it is still difficult to accurately design SACs with high activity and specific selectivity due to the complicated combinations of metal atoms and substrates.…”

Section: Introductionmentioning

confidence: 99%

Interpretable Machine Learning‐Assisted High‐Throughput Screening for Understanding NRR Electrocatalyst Performance Modulation between Active Center and C‐N Coordination

Sun,

Chen,

Guan

et al. 2023

Energy & Environ Materials

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Understanding the correlation between the fundamental descriptors and catalytic performance is meaningful to guide the design of high‐performance electrochemical catalysts. However, exploring key factors that affect catalytic performance in the vast catalyst space remains challenging for people. Herein, to accurately identify the factors that affect the performance of N2 reduction, we apply interpretable machine learning (ML) to analyze high‐throughput screening results, which is also suited to other surface reactions in catalysis. To expound on the paradigm, 33 promising catalysts are screened from 168 carbon‐supported candidates, specifically single‐atom catalysts (SACs) supported by a BC3 monolayer (TM@VB/C‐Nn = 0–3‐BC3) via high‐throughput screening. Subsequently, the hybrid sampling method and XGBoost model are selected to classify eligible and non‐eligible catalysts. Through feature interpretation using Shapley Additive Explanations (SHAP) analysis, two crucial features, that is, the number of valence electrons (Nv) and nitrogen substitution (Nn), are screened out. Combining SHAP analysis and electronic structure calculations, the synergistic effect between an active center with low valence electron numbers and reasonable C‐N coordination (a medium fraction of nitrogen substitution) can exhibit high catalytic performance. Finally, six superior catalysts with a limiting potential lower than −0.4 V are predicted. Our workflow offers a rational approach to obtaining key information on catalytic performance from high‐throughput screening results to design efficient catalysts that can be applied to other materials and reactions.

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Section: Introductionmentioning

confidence: 99%

Interpretable Machine Learning‐Assisted High‐Throughput Screening for Understanding NRR Electrocatalyst Performance Modulation between Active Center and C‐N Coordination

Sun,

Chen,

Guan

et al. 2023

Energy & Environ Materials

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“…To clearly illustrate the change of the crystal orbital, we calculate the crystal orbital Hamilton population (COHP) and the integrated COHP (ICOHP) − for intrinsic C 2 N and C 2 NSi. Figure S2 exhibits the bonding characteristics of the C–N π* antibonding orbital and the C–C σ bonding orbital.…”

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confidence: 99%

Metal-Free Carbon Nitride Nanosheet Supported the Pentacoordinated Silicon Intermediates for Photocatalytic Overall Water Splitting

Shi

Sun

Guan

et al. 2023

J. Phys. Chem. Lett.

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Photocatalytic overall water splitting is a promising approach to overcome the environmental and energy crisis. However, developing effective photocatalysts with well activity, light absorption, and photogenerated carrier lifetime is still a challenge. Herein, combining extensive first-principles and nonadiabatic molecular dynamics calculations, we find that microporous carbonnitride nanosheets with a pyridinic nitrogen, such as C 2 N and C 6 N 6 , possess the pentacoordinated silicon intermediates' bonding environment. The pentacoordinated silicon as intermediates exhibits good photocatalytic performance for the difficult four-electronic oxygen evolution reaction. The overpotential is only 0.55 V for C 2 N, which is significantly lower than that of the tetracoordinated silicon intermediates (2.00 V). Simultaneously, the decoration of the silicon group not only widens the absorption range of visible light but also maintains the lifetime of photogenerated carriers on the nanosecond scale, which enhances the application efficiency of solar energy. Our work paves a new route for advancing photocatalytic overall water splitting.

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N2 reduction to NH3 on surfaces of Co-Al18P18, Ni-Al21N21, Fe-B24N24, Mn-B27P27, Ti-C60 and Cu-Si72 catalysts

Hsu,

Mustafa,

Yadav

et al. 2024

J Mol Model

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Theoretical exploration of the nitrogen fixation mechanism of two-dimensional dual-metal TM₁TM₂@C₉N₄ electrocatalysts

Abstract: Electrochemical nitrogen reduction reaction (eNRR) to NH3 has become an alternative to the traditional NH3 production technique, while developing NRR catalysts with high activity and high selectivity is of great...

Cited by 12 publications

References 50 publications

Interpretable Machine Learning‐Assisted High‐Throughput Screening for Understanding NRR Electrocatalyst Performance Modulation between Active Center and C‐N Coordination

Interpretable Machine Learning‐Assisted High‐Throughput Screening for Understanding NRR Electrocatalyst Performance Modulation between Active Center and C‐N Coordination

Metal-Free Carbon Nitride Nanosheet Supported the Pentacoordinated Silicon Intermediates for Photocatalytic Overall Water Splitting

N2 reduction to NH3 on surfaces of Co-Al18P18, Ni-Al21N21, Fe-B24N24, Mn-B27P27, Ti-C60 and Cu-Si72 catalysts

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