A DFT-based study of As2O3 adsorption using single and bimetallic atom-doped g-C3N4

IF 2.9 3区化学 Q3 CHEMISTRY, PHYSICAL

Physical Chemistry Chemical Physics Pub Date : 2025-09-30 DOI:10.1039/d5cp02303c

Jialiang Sun, Xiantuo Chen, Shun Liu, Dapeng Wang, Min Li, Guangqian Luo, Hong Yao, Jiang Wu, Qizhen Liu

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Abstract

Non-precious metal atom-doped g-C₃N₄ is a promising adsorbent for arsenic removal from coal-fired flue gas, but the adsorption process and mechanisms are unclear. This work systematically investigates As₂O₃ adsorption on single- and double-transition-metal-loaded g-C₃N₄ using density functional theory, examining the adsorption location, structure, energy, and charge density. Calculations show that metal doping significantly improves As₂O₃ adsorption capacity. Adsorption energy on M₂/g-C₃N₄ (where M₂ denotes a bimetallic atom) exceeds that on M/g-C₃N₄ (where M denotes a monometallic atom) due to bimetallic atoms' synergistic and electronic effects. Co₂ introduction has the most obvious effect, with an adsorption energy of −565.1 kJ mol⁻¹—4.36 and 2.25 times higher than that of pure g-C₃N₄ and monoatomic Co doping, respectively. This indicates that bimetallic doping favors As₂O₃ adsorption. Projected density of states and adsorption process analysis further verify the excellent performance of bimetallic-doped g-C₃N₄. This DFT study contributes to understanding the atomic-scale adsorption mechanism and aids in the rational design of high-performance adsorbents.

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单金属和双金属原子掺杂g-C3N4吸附As2O3的dft研究

非贵金属原子掺杂g-C3N4是一种很有前途的燃煤烟气除砷吸附剂，但其吸附过程和机理尚不清楚。本文利用密度泛函理论系统地研究了As2O3在单和双过渡金属负载g-C3N4上的吸附，考察了吸附位置、结构、能量和电荷密度。计算表明，金属掺杂显著提高了As2O3的吸附能力。M2/g-C3N4 （M2为双金属原子）上的吸附能大于M/g-C3N4 （M为单金属原子）上的吸附能，这是由于双金属原子的协同效应和电子效应。引入Co2的效果最明显，吸附能为- 565.1 kJ mol - 1-4.36倍，比纯g-C3N4和单原子Co掺杂分别高2.25倍。这表明双金属掺杂有利于吸附As2O3。投影态密度和吸附过程分析进一步验证了双金属掺杂g-C3N4的优异性能。该研究有助于理解原子尺度的吸附机理，有助于高效吸附剂的合理设计。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Physical Chemistry Chemical Physics 化学-物理：原子、分子和化学物理

CiteScore

5.50

自引率

9.10%

发文量

2675

审稿时长

2.0 months

期刊介绍： Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.