非对称CoN1C2配位的高自旋构型促进类芬顿反应中d-p轨道杂化

doi:10.1016/S1872-2067(25)64674-2

催化学报 ›› 2025, Vol. 73: 334-346.DOI: 10.1016/S1872-2067(25)64674-2

非对称CoN₁C₂配位的高自旋构型促进类芬顿反应中d-p轨道杂化

白倩^a, 齐娟娟^a(), 张荣哲^a, 陈志远^b, 魏子皓^c, 孙志一^c, 邓紫微^c, 杨旭东^a, 李蔷薇^a, 陈文星^c, 汪黎东^a()

^a华北电力大学环境科学与工程学院, 资源与环境系统优化教育部重点实验室, 北京 102206, 中国
^b华威大学统计系, 考文垂, 英国
^c北京理工大学材料科学与工程学院, 能源与催化中心, 北京 100081, 中国

收稿日期:2024-12-24 接受日期:2025-03-19 出版日期:2025-06-18 发布日期:2025-06-12
通讯作者: *电子信箱: qijuanjuan@ncepu.edu.cn (齐娟娟),wld@ncepu.edu.cn (汪黎东).
基金资助:
国家杰出青年科学基金(52325004);国家自然科学基金(51878273);国家自然科学基金(22375019);国家自然科学基金(22106045);河北省科学院科技计划项目(25A04);河北省科学院科技计划项目;本研究还得到了华北电力大学高性能计算平台的支持

High-spin configuration of asymmetric CoN₁C₂ coordination for boosting d-p orbital hybridization in Fenton-like reactions

Qian Bai^a, Juanjuan Qi^a(), Rongzhe Zhang^a, Zhiyuan Chen^b, Zihao Wei^c, Zhiyi Sun^c, Ziwei Deng^c, Xudong Yang^a, Qiangwei Li^a, Wenxing Chen^c, Lidong Wang^a()

^aMOE Key Laboratory of Resources and Environmental Systems Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China
^bDepartment of Statistics, University of Warwick, Coventry, UK
^cEnergy & Catalysis Center, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China

Received:2024-12-24 Accepted:2025-03-19 Online:2025-06-18 Published:2025-06-12
Contact: *E-mail: qijuanjuan@ncepu.edu.cn (J. Qi),wld@ncepu.edu.cn (L. Wang).
Supported by:
National Science Fund for Distinguished Young Scholars(52325004);National Natural Science Foundation of China(51878273);National Natural Science Foundation of China(22375019);National Natural Science Foundation of China(22106045);Science and Technology Program Project(25A04) of Hebei Academy of Sciences,);Science and Technology Program Project;high-performance computing platform of North China Electric Power University

摘要/Abstract

摘要：

传统污水处理工艺在去除痕量浓度的新兴有机污染物(如活性药物)方面具有一定的局限性, 亟需开发高效的深度处理工艺以满足日益严格的排放要求. 目前, 非均相类芬顿工艺因其显著的去除效率展现出广阔的应用前景. 然而, 催化剂的设计仍是推动该工艺发展的关键因素. 近年来, 非对称单原子催化剂(ASACs)因其优异的催化性能而受到广泛关注, 但如何实现高金属负载, 精准调控自旋态以及阐明配位环境与催化性能之间的关系等方面仍面临挑战. 因此, 设计具有高自旋构型和非对称配位的催化剂, 有望通过促进类芬顿反应中d-p轨道杂化, 提升污染物降解效率, 从而推动高级氧化技术的发展.

本文通过原位生成碳缺陷的方法, 成功设计了高负载钴的ASACs (CoN₁C₂/C₂N), 其将钴单原子锚定在三维花状结构的C₂N基底上. 采用X射线吸收精细结构和高角度环形暗场扫描透射电子显微镜对催化剂的非对称配位和单原子形貌进行了确认. 通过M-T曲线拟合和密度泛函理论计算揭示了由于非对称配位的引入Co活性位点的电子自旋态从低自旋态(LS, t_2g⁶e_g¹)转变为高自旋态(HS, t_2g⁵e_g²). 与对称结构的CoN₂/C₂N催化剂中Co 3d未配对电子n ≈ 1相比, CoN₁C₂/C₂N中Co 3d具有更多的未配对电子(n ≈ 3), 这使其表现出更强的从HSO₅^-的O 2p轨道获取电子的能力, 进而促进了类芬顿反应中的d-p轨道杂化. 实验结果表明, 优化后的CoN₁C₂/C₂N在医药废水深度氧化处理中表现出卓越的催化活性, 3 min内通过活化过一硫酸盐(PMS)实现对磺胺氯哒嗪钠(SCP)的降解效率达到100%, 周转频率值为36.8 min^-1, 与现有催化剂相比展示出优异的催化活性. 此外, 该催化剂在宽pH范围内以及阴阳离子共存条件下, 降解效果几乎不受影响, 显示出较好的普适性. 通过对不同反应体系降解机制的研究, 结果表明, 不同的基底会选择性生成不同的活性氧物种(ROSs). 当负载基底为C₂N时, 体系中主要ROSs为单线态氧(¹O₂)为主; 而当负载基底为C₃N₄时, 主要ROSs包括羟基自由基(^•OH), 硫酸根自由基(SO₄^•−)和 ¹O₂. 进一步理论计算结果证实, 当催化剂CoN₁C₂/C₂N与PMS作用时, 具有高自旋构型的HS Co 3d-O 2p的σ*轨道中的自旋电子填充加速了 ^*SO₅^•−的脱附, 该过程为反应动力学中的限速步骤, 从而促进了更多 ¹O₂生成, 最终实现了高效的催化效果.

综上所述, 本文报道了具有高自旋构型和非对称配位的CoN₁C₂/C₂N催化剂在活化PMS降解SCP方面的优异性能, 并深入探究了其机理. 系统研究了在非均相类芬顿反应体系中, 高效的d-p轨道杂化是提升催化性能的关键. 本研究不仅为非对称配位与金属位点自旋态之间的关系提供了宝贵的见解, 还阐明了σ*轨道在ROSs生成中的重要作用, 为环境修复和能源转化领域的应用发展提供了新思路.

关键词: 非对称配位, C₂N, 高自旋构型, d-p轨道杂化, 类芬顿反应

Abstract:

Asymmetric single-atom catalysts (ASACs) have attracted much attention owing to their excellent catalytic properties. However, the relationship between asymmetric coordination and the spin states of metal sites remains unclear. Additionally, the modulation of reactive oxygen species in Fenton-like reactions remains challenging. Herein, a novel strategy is reported for the rational design of highly loaded Co ASACs (CoN₁C₂/C₂N) immobilized on three-dimensional flower-like C₂N using an in situ-generated carbon defect method. In particular, the asymmetrically tricoordinated CoN₁C₂/C₂N exhibited excellent catalytic activity for sulfachloropyridazine degradation, with a turnover frequency of 36.8 min^-1. Experimental results and theoretical calculations revealed that the electron spin state of the Co-active sites was transferred from the low-spin configuration (t_2g⁶e_g¹) to the high-spin configuration (t_2g⁵e_g²) owing to asymmetric coordination. The high-spin Co 3d orbital in CoN₁C₂/C₂N possessed more unpaired electrons and therefore, had a strong ability to gain electrons from the O 2p orbitals of HSO₅^-, boosting d-p orbital hybridization. More importantly, the spin-electron filling in the σ* orbital of high-spin Co 3d−O 2p accelerated the desorption of ^*SO₅^•−, which acted as a rate-limiting step in the reaction, thus facilitating more ¹O₂ generation. This study provides an innovative synthetic route for practical ASACs and clarifies the critical relationship between structure and spin state, paving the way for advancements in environmental remediation and energy conversion applications.

Key words: Asymmetric coordination, C₂N, High-spin configuration, d-p orbital hybridization, Fenton-like reaction

白倩, 齐娟娟, 张荣哲, 陈志远, 魏子皓, 孙志一, 邓紫微, 杨旭东, 李蔷薇, 陈文星, 汪黎东. 非对称CoN₁C₂配位的高自旋构型促进类芬顿反应中d-p轨道杂化[J]. 催化学报, 2025, 73: 334-346.

Qian Bai, Juanjuan Qi, Rongzhe Zhang, Zhiyuan Chen, Zihao Wei, Zhiyi Sun, Ziwei Deng, Xudong Yang, Qiangwei Li, Wenxing Chen, Lidong Wang. High-spin configuration of asymmetric CoN₁C₂ coordination for boosting d-p orbital hybridization in Fenton-like reactions[J]. Chinese Journal of Catalysis, 2025, 73: 334-346.

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https://www.cjcatal.com/CN/Y2025/V73/I6/334

图/表 6

Fig. 1. Synthesis and characterization of CoN1C2/C2N. (a) Schematic illustration of the synthesis of CoN1C2/C2N. (b) SEM images of CoN1C2/C2N. (c) TEM image of CoN1C2/C2N showing the 2D sheet structure. (d) Element-mapping of CoN1C2/C2N. (e) HAADF-STEM image of CoN1C2/C2N. (f) The enlarged image of the yellow area in (e) shows that single atoms are dispersed on C2N. (g) 3D model of isolated single-Co atoms (seen as bright spots) and corresponding intensity profiles along the red dotted line in (f).

Fig. 2. Electronic structure of CoN1C2/C2N. (a) Soft XANES spectrum of the C K side of CoN1C2/C2N. (b) Soft XANES spectrum of the N K side of CoN1C2/C2N. (c) Co K-edge XANES spectra of CoN1C2/C2N and the three comparison samples. (d) FT-EXAFS spectra of CoN1C2/C2N and the remaining three comparison samples. (e) WT analysis of EXAFS signaling spectra. (f) FT-EXAFS fitting curve of CoN1C2/C2N in K-space. (g) FT-EXAFS fitting curve of CoN1C2/C2N in R-space. (h) Atomic structure model of CoN1C2/C2N.

Fig. 3. Spin state of CoN1C2/C2N and CoN2/C2N. (a) XPS fine spectra of C 1s. (b) XPS fine spectra of N 1s. (c) XPS fine spectra of Co 2p. (d) M-T curves of CoN1C2/C2N and CoN2/C2N. (e) Schematic representation of the spin transition of Co with different coordination environments. (f) Co L-edge XANES spectra of CoN1C2/C2N and CoN2/C2N. (g) The PDOS of CoN1C2/C2N and CoN2/C2N. (h) CDD of CoN1C2/C2N.

Fig. 4. Fenton-like properties of CoN1C2/C2N. (a) Degradation of SCP in different catalytic systems. (b) k1 values of SCP in different catalytic systems. (c) Effect of initial pH. (d) Effects of adding anions, cations, or NOM to CoN1C2/C2N/PMS systems on SCP degradation within 3 min. (e) Pollutant removal efficiencies of the current and other recently reported catalysts versus PMS dosage. (f) Degradation k1 values of different pollutants in CoN1C2/C2N/PMS system and structural formula of organics. (g) Correlation between the corresponding k1 values and the N index. (h) Cyclic and regenerative properties of CoN1C2/C2N/PMS system for SCP removal. Reaction condition: [catalyst] = 0.1 g L-1, [PMS] = 0.1 g L-1, [Pollutants] = 20.0 mg L-1, [anions and cation] = 1 mmol L-1, [HA] = 1 mM, and initial pH = 7.0-10.5±0.2.

Fig. 5. Detection of active substances of three catalysts. (a) Quenching experiments in CoN1C2/C2N/PMS system. (b) Quenching experiments in CoN2/C3N4/PMS system. (c) Removal efficiency of different quenchers in different PMS systems after 3 min. (d) EPR spectra of SO4?? and ?OH. (e) EPR spectra of 1O2. (f) An overview of the relationship among substrate, ROS, coordination environment, spin state, and catalytic properties. Reaction condition: [catalyst] = 0.1 g L-1, [PMS] = 0.1 g L-1, [Pollutants] = 20.0 mg L-1, [MeOH, TBA] = 200 mmol L-1, [L-histidine] = 5 mmol L-1, and initial pH = 7.0±0.2.

Fig. 6. DFT calculations and data analysis of the catalysts before and after reaction. (a) CDD, adsorption energy, and number of transferred electrons after PMS adsorption. (b) Schematic diagram of electron transfer ability in different coordination environments. (c) Orbital interactions between HSO5? and single-atom Co catalysts. (d) XPS of CoN1C2/C2N catalyst after reaction. (e) Free energy of different coordination structures. (f) XRD patterns of the CoN1C2/C2N catalyst after reaction.

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非对称CoN₁C₂配位的高自旋构型促进类芬顿反应中d-p轨道杂化

High-spin configuration of asymmetric CoN₁C₂ coordination for boosting d-p orbital hybridization in Fenton-like reactions

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