DFT and machine learning study of oxygen-doped two-dimensional borophene catalyzed oxidative dehydrogenation of benzylamine

SI Chaowei; ZHAN Jie; XU Wenjing; LI Bo; CHEN Xingqiu

doi:10.11949/0438-1157.20260474

您当前的位置：

首页 >

文章列表页 >

DFT and machine learning study of oxygen-doped two-dimensional borophene catalyzed oxidative dehydrogenation of benzylamine

更新时间：2026-05-18

- DFT and machine learning study of oxygen-doped two-dimensional borophene catalyzed oxidative dehydrogenation of benzylamine
- CIESC Journal (2026)
- 作者机构：
  
  1.中国科学技术大学材料科学与工程学院，辽宁沈阳 110016
  2.中国科学院金属研究所，辽宁沈阳 110016
  3.沈阳师范大学化学化工学院，辽宁沈阳 110034
- 作者简介：
- 基金信息：
- DOI：10.11949/0438-1157.20260474
  CLC： TQ 032.4
- Received：07 April 2026，
  
  Revised：2026-05-17，
  
  Accepted：18 May 2026，
- 稿件说明：
移动端阅览
SI Chaowei, ZHAN Jie, XU Wenjing, et al. DFT and machine learning study of oxygen-doped two-dimensional borophene catalyzed oxidative dehydrogenation of benzylamine[J/OL]. CIESC Journal, 2026.
DOI：

SI Chaowei, ZHAN Jie, XU Wenjing, et al. DFT and machine learning study of oxygen-doped two-dimensional borophene catalyzed oxidative dehydrogenation of benzylamine[J/OL]. CIESC Journal, 2026. DOI： 10.11949/0438-1157.20260474.

摘要

本文基于密度泛函理论，研究了氧掺杂量与掺杂位点对二维硼烯结构及性能的影响。计算结果表明，适量氧掺杂能够优化硼烯几何与电子结构，促进苄胺的高效吸附与低能垒脱氢。其中，最上层氧掺杂量达33 wt%的二维硼烯催化剂活性最佳，其催化苄胺氧化脱氢能垒仅为0.33 eV，且过度脱氢副反应的能垒高达3.17 eV，表明该催化剂对目标产物苯甲亚胺具有高选择性。基于机器学习方法构建的预测模型成功预测了不同取代基底物的性能趋势，模型揭示的第一步脱氢能垒为最关键描述符。本研究结合理论计算与机器学习模型，系统阐明了氧掺杂硼烯催化剂的构效关系，为设计高效低维纳米催化体系提供了理论依据。

Abstract

Using density functional theory (DFT)

the effects of different doping amounts and doping sites on oxygen-doped two-dimensional borophene were systematically investigated. The calculation results show that an appropriate amount of oxygen doping can optimize the geometric and electronic structures of borophene

enabling efficient adsorption of benzylamine and low-energy-barrier dehydrogenation. The oxygen-doped two-dimensional borophene catalyst with 33 wt% oxygen doping on the top layer exhibits the best catalytic activity

with an energy barrier of only 0.33 eV for the oxidative dehydrogenation of benzylamine and an energy barrier as high as 3.17 eV for the over-dehydrogenation side reaction

indicating its high selectivity toward the target product

benzylideneimine. A prediction model based on machine learning successfully predicted the performance trends of substrates with different substituents

and the model revealed that the first-step dehydrogenation energy barrier is the most critical descriptor. By combining theoretical calculations and machine learning predictions

this study systematically elucidates the structure–activity relationship of oxygen-doped borophene catalysts

providing a complete theoretical framework for the rational design of efficient non-noble metal catalytic systems.

关键词

Keywords

references

Wu B H , Li X Y , Hou T L , et al . Oxygen-bridged Cu and V dual metal sites for enhanced photo-oxidative coupling of benzylamine [J ] . Journal of the American Chemical Society , 2025 , 147 ( 51 ): 46997 - 47007 .

Daems N , Sheng X , Vankelecom I F J , et al . Metal-free doped carbon materials as electrocatalysts for the oxygen reduction reaction [J ] . Journal of Materials Chemistry A , 2014 , 2 ( 12 ): 4085 - 4110 .

Tang C X , Bao T F , Li S M , et al . Rapid charge transfer endowed by hollow-structured Z-scheme heterojunction for coupling benzylamine oxidation with CO 2 reduction [J ] . Advanced Functional Materials , 2024 , 35 ( 7 ): 2415280 .

Wen X X , Prezhdo O V , Xu L . Design of twisted two-dimensional heterostructures and performance regulation descriptor for electrocatalytic ammonia production from nitric oxide [J ] . Journal of the American Chemical Society , 2025 , 147 ( 17 ): 14647 - 14658 .

Sheng S X , Wu J B , Cong X , et al . Raman spectroscopy of two-dimensional borophene sheets [J ] . ACS Nano , 2019 , 13 ( 4 ): 4133 - 4139 .

Santos-Putungan A B , Herrera M U , Putungan D B . Atomic hydrogen adsorption on freestanding α-borophene nanoribbons for hydrogen spillover applications: insights from density functional theory calculations [J ] . Journal of Physics: Conference Series , 2023 , 2543 ( 1 ): 012012 .

Li C Y , Liu X , Wu D D , et al . Theoretical study of transition metal doped α-borophene nanosheet as promising electrocatalyst for electrochemical reduction of N 2 [J ] . Computational and Theoretical Chemistry , 2022 , 1213 : 113732 .

Mannix A J , Zhou X F , Kiraly B , et al . Synthesis of borophenes: Anisotropic, two-dimensional boron polymorphs [J ] . Science , 2015 , 350 ( 6267 ): 1513 - 1516 .

Qin X M , Yan W J , Li D X , et al . A first-principles study of gas molecule adsorption on carbon-, nitrogen-, and oxygen-doped two-dimensional borophene [J ] . Advances in Condensed Matter Physics , 2021 , 2021 ( 1 ): 3760631 .

Gu Q Q , Lin H J , Si C W , et al . Tuning the active oxygen species of two-dimensional borophene oxide toward advanced metal-free catalysis [J ] . ACS Nano , 2024 , 18 ( 44 ): 30574 - 30583 .

Mabhulusa W , Sekhosana K E , Fuku X . Incorporation of Pd catalyst into highly effective borophene nanosheet co-catalyst for electrokinetics and electrochemical oxygen reduction reactions [J ] . Journal of Electronic Materials , 2024 , 53 ( 7 ): 4236 - 4249 .

Mortazavi B , Dianat A , Rahaman O , et al . Borophene as an anode material for Ca, Mg, Na or Li ion storage: a first-principle study [J ] . Journal of Power Sources , 2016 , 329 : 456 - 461 .

Liu M L , Rao F , Liao M Q , et al . Screening of borophene-supported highly active and selective single-atom catalysts for electrocatalytic nitrogen reduction reactions [J ] . Applied Materials Today , 2024 , 38 : 102166 .

Zheng Y N , Chen W X , Liu Z K , et al . Tri-coordinated boron species in confined boron oxide catalysts for enhanced low-temperature oxidative dehydrogenation of propane [J ] . Angewandte Chemie International Edition , 2025 , 64 ( 28 ): e202507525 .

Liu Y M , Feng W L , Li T C , et al . Structure and catalytic properties of vanadium oxide supported on mesocellulous silica foams (MCF) for the oxidative dehydrogenation of propane to propylene [J ] . Journal of Catalysis , 2005 , 239 ( 1 ): 125 - 136 .

Grant J T , Love A M , Carrero C A , et al . Improved supported metal oxides for the oxidative dehydrogenation of propane [J ] . Topics in Catalysis , 2016 , 59 ( 17-18 ): 1545 - 1553 .

Lu W D , Gao X Q , Wang Q G , et al . Ordered macroporous boron phosphate crystals as metal-free catalysts for the oxidative dehydrogenation of propane [J ] . Chinese Journal of Catalysis , 2020 , 41 ( 12 ): 1837 - 1845 .

Arnold F M , Seifert G , Kunstmann J . Thermodynamic stability of borophene, B 2 O 3 and other B 1– x O x sheets [J ] . Journal of Physics Communications , 2020 , 4 ( 3 ): 031001 .

Feng B , Sugino O , Liu R Y , et al . Dirac fermions in borophene [J ] . Physical Review Letters , 2017 , 118 ( 9 ): 096401 .

Fazilaty M , Pourahmadi M , Shayesteh M R , et al . Investigating and comparing structural, electronic and optical properties of χ 3 -borophene in monolayer, nanoribbon and nanotube modes as a transparent metal [J ] . Journal of Physics and Chemistry of Solids , 2021 , 148 : 109683 .

Guo R Y , Li T , Shi S E , et al . Oxygen defects formation and optical identification in monolayer borophene [J ] . Materials Chemistry and Physics , 2017 , 198 : 346 - 353 .

罗文崴 . 硼烯的抗氧化性能及其电子特性调控的理论研究 [D ] . 南昌 : 江西师范大学 , 2020 .Luo W W. Theoretical study on anti-oxidation and electronic properties regulation of borophene. Nanchang: Jiangxi Normal University , 2020.

Alvarez-Quiceno J C , Miwa R H , Dalpian G M , et al . Oxidation of free-standing and supported borophene [J ] . 2D Materials , 2017 , 4 ( 2 ): 025025 .

Kresse G , Hafner J . Ab initio molecular dynamics for liquid metals [J ] . Physical Review B , 1993 , 47 ( 1 ): 558 - 561 .

Kresse G , Furthmüller J . Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set [J ] . Computational Materials Science , 1996 , 6 ( 1 ): 15 - 50 .

Blöchl P E . Projector augmented-wave method [J ] . Physical Review B , 1994 , 50 ( 24 ): 17953 - 17979 .

Kresse G , Joubert D . From ultrasoft pseudopotentials to the projector augmented-wave method [J ] . Physical Review B , 1999 , 59 ( 3 ): 1758 - 1775 .

Hammer B , Hansen L B , Nørskov J K . Improved adsorption energetics within density-functional theory using revised Perdew-Burke-Ernzerhof functionals [J ] . Physical Review B , 1999 , 59 ( 11 ): 7413 - 7421 .

Grimme S , Ehrlich S , Goerigk L . Effect of the damping function in dispersion corrected density functional theory [J ] . Journal of Computational Chemistry , 2011 , 32 ( 7 ): 1456 - 1465 .

Kistanov A A , Khadiullin S K , Dmitriev S V , et al . Effect of oxygen doping on the stability and band structure of borophene nanoribbons [J ] . Chemical Physics Letters , 2019 , 728 : 53 - 56 .

Lu B Q , Zheng Z W , Liu T Z , et al . A global optimization algorithm based on multi-loop neural network control [J ] . Journal of Systems Engineering and Electronics , 2019 , 30 ( 5 ): 1007 .

Chen S F . K-nearest neighbor algorithm optimization in text categorization [J ] . IOP Conference Series: Earth and Environmental Science , 2018 , 108 ( 5 ): 052074 .

Friedman J H . Stochastic gradient boosting [J ] . Computational Statistics & Data Analysis , 2002 , 38 ( 4 ): 367 - 378 .

Breiman L . Random forests [J ] . Machine Learning , 2001 , 45 ( 1 ): 5 - 32 .

林梦 , 周顺利 , 张成喜 , 等 . 固体酸烷基化催化剂低温高效再生工艺优化 [J ] . 当代化工 , 2025 , 154 ( 9 ): 2029 - 2034+2068 .

Lin M , Zhang C X , Zhou S L , et al . Optimization of low-temperature high-efficiency regeneration process for solid acid alkylation catalysts [J ] . 当代化工 , 2025 , 54 ( 09 ): 2029 - 2034+2068 .

雷亮 . A110型氨合成催化剂的还原与探讨 [J ] . 中氮肥 , 2004 ( 2 ): 19 - 22 .

Lei L . Disscussion on the reduction of A110 ammonia synthesis catalyst [J ] . M-Sized Nitrogenous Fertilizer Progress , 2004 ( 2 ): 19 - 22 .

胡庆敏 . 高效纳米催化剂及气体传感器的设计与制备: 原子层沉积与界面调控 [D ] . 上海 : 上海大学 , 2021 .

Hu Q M . High-performance nanocatalysts and gas sensors design with atomic layer deposition and interface tailoring [D ] . Shanghai : Shanghai University , 2021 .

Views

下载量

CSCD

Alert me when the article has been cited

提交

Tools

Publicity Resources

Research progress on persulfate-based advanced oxidation technology regulated by chelating agents

Boosting persulfate activation via carbon dots-mediated Cu²⁺/Cu⁺ redox cycling under visible light for efficient tetracycline removal

Preparation of nanoscale zero-valent iron and its application of reduction and oxidation technology

Progress on stability enhancement of black phosphorene

Recent advances in machine learning for modeling and control of crystallization processes

Related Author

XIE Songru

CHEN Haoyun

YUAN Xingzhong

JIANG Longbo

PANG Ernan

LI Shijia

LUO Zhili

LI Ruyue

Related Institution

School of Resource and Environment, Hunan University of Technology and Business

Xiang Jiang Laboratory

College of Environmental Science and Engineering, Hunan University

Institute of Traffic Engineering, Shanxi Vocational University of Engineering Science and Technology

College of Safety and Environmental Engineering, Shandong University of Science and Technology

⁰