外围氮空位诱导电子传递至Fe单原子以实现高效的氧气活化过程

doi:10.1016/S1872-2067(25)64651-1

催化学报 ›› 2025, Vol. 72: 187-198.DOI: 10.1016/S1872-2067(25)64651-1

外围氮空位诱导电子传递至Fe单原子以实现高效的氧气活化过程

刘粉利^a^,¹, 杨曼^b^,¹, 段江林^a, 殷祉钰^a, 史名扬^a, 陈馥清^a, 熊惠峰^a, 刘忻^c, 刘文刚^e, 夏琦兴^f, 孙少东^b, 冯丹^g, 齐海峰^d^,^*(), 覃勇^e^,^h^,^*(), 任煜京^a^,ⁱ^,^*()

^a西北工业大学生命学院, 生物与催化交叉研究中心, 陕西西安 710072, 中国
^b西安理工大学, 材料科学与工程学院, 陕西西安 710048, 中国
^c东北大学秦皇岛分校, 资源与材料学院, 河北秦皇岛 066004, 中国
^d卡迪夫大学, 马克斯·普朗克-卡迪夫多相催化基础研究中心, 卡迪夫, 英国
^e青岛科技大学, 材料科学与工程学院, 山东青岛 266042, 中国
^f西北工业大学, 文化遗产研究院, 陕西西安 710072, 中国
^g西北工业大学, 分析测试中心, 陕西西安 710072, 中国
^h中国科学院山西煤炭化学研究所, 煤炭高效低碳利用全国重点实验室, 山西太原 030001, 中国
ⁱ西北工业大学重庆科创中心, 重庆 401135, 中国
^j西北工业大学深圳研究院, 广东深圳 518057, 中国

收稿日期:2024-12-11 接受日期:2025-03-01 出版日期:2025-05-18 发布日期:2025-05-20
通讯作者: *电子信箱: qih11@cardiff.ac.uk (齐海峰),qinyong@qust.edu.cn (覃勇),renyj@nwpu.edu.cn (任煜京).
作者简介:¹共同第一作者.
基金资助:
国家重点研发项目(2023YFA1506603);国家自然科学基金(22472131);国家自然科学基金(22478316);国家自然科学基金(22208262);国家自然科学基金(52101272);国家自然科学基金(52271228);重庆市自然科学基金(CSTB2023NSCQ-MSX0165);广东省基础与应用基础研究基金(2024A1515012109);山东省自然科学基金(ZR2021YQ09);泰山学者工程专项基金(tsqn202312200);煤炭高效低碳利用全国重点实验室开放课题(J24-25-903);欧盟玛丽·居里基金(101107009-AtomCat4Fuel);英国国家科研与创新署UKRI基金(EP/Y029305/1)

Peripheral N_V-induced electron transfer to Fe₁ single atoms for highly efficient O₂ activation

Fenli Liu^a^,¹, Man Yang^b^,¹, Jianglin Duan^a, Zhiyu Yin^a, Mingyang Shi^a, Fuqing Chen^a, Huifeng Xiong^a, Xin Liu^c, Wengang Liu^e, Qixing Xia^f, Shaodong Sun^b, Dan Feng^g, Haifeng Qi^d^,^*(), Yong Qin^e^,^h^,^*(), Yujing Ren^a^,ⁱ^,^*()

^aInterdisciplinary Research Center of Biology & Catalysis, School of Life Sciences, Northwestern Polytechnical University, Xi’an 710072, Shaanxi, China
^bSchool of Materials Science and Engineering, Xi’an University of Technology, Xi’an 710048, Shaanxi, China
^cSchool of Resources and Materials, Northeastern University at Qinhuangdao, Qinhuangdao 066004, Hebei, China
^dMax Planck-Cardiff Centre on the Fundamentals of Heterogeneous Catalysis FUNCAT, Translational Research Hub, Cardiff University, Maindy Road, Cardiff CF24 4HQ, UK.
^eCollege of Materials Science and Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China
^fInstitute of Culture and Heritage, Northwestern Polytechnical University, Xi’an 710072, Shaanxi, China
^gAnalytical & Testing Center, Northwestern Polytechnical University, Xi’an 710072, Shaanxi, China
^hState Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi, China
ⁱChongqing Innovation Center, Northwestern Polytechnical University, Chongqing 401135, China
^jShenzhen Research Institute of Northwestern Polytechnical University, Shenzhen 518057, Guangdong, China

Received:2024-12-11 Accepted:2025-03-01 Online:2025-05-18 Published:2025-05-20
Contact: *E-mail: qih11@cardiff.ac.uk (H. Qi), qinyong@qust.edu.cn (Y. Qin), renyj@nwpu.edu.cn (Y. Ren).
About author:¹ Contributed equally to this work.
Supported by:
National Key R&D Program of China(2023YFA1506603);National Natural Science Foundation of China(22472131);National Natural Science Foundation of China(22478316);National Natural Science Foundation of China(22208262);National Natural Science Foundation of China(52101272);National Natural Science Foundation of China(52271228);Natural Science Foundation of Chongqing China(CSTB2023NSCQ-MSX0165);Guangdong Basic and Applied Basic Research Foundation(2024A1515012109);Natural Science Foundation of Shandong Province(ZR2021YQ09);Taishan Scholars Project Special Funds(tsqn202312200);Foundation of State Key Laboratory of Coal Conversion(J24-25-903);Marie Skłodowska-Curie Actions Postdoctoral Fellowships(101107009-AtomCat4Fuel);UKRI(EP/Y029305/1)

摘要/Abstract

摘要：

催化氧化作为现代化学工业中的基本反应过程之一, 在能源转化、化学品合成及环境保护领域具有重要意义. 其中, 将有机分子中广泛存在的C-H/C-O/C-N键选择性氧化为更高价值的官能团, 已成为精细化学品合成中重要的反应之一. 上述反应在传统上主要依赖于过氧化物、卤素及臭氧等氧化剂. 相比之下, 使用氧气(O₂)作为氧化剂则兼具生态友好性与原子经济性的优势. 截至目前, 现有高性能反应体系主要为贵金属基催化剂. 特别是针对惰性C-H键的氧化活化, 开发高效的非贵金属基催化剂仍面临重大挑战.

自然界中, 具有细胞色素P-450 (CTY-P450)结构的黄素依赖单加氧酶能在温和条件下通过Fe₁-卟啉(血红素)位点高效催化O₂转化为活性氧物种. 值得注意的是, 在此呼吸链过程中, 含氮杂环化合物(如NAD(P)H/NAD(P)+和还原/氧化态黄素)充当激发电子供体. 受此启发, 通过在具有与NAD(P)H及黄素化合物活性单元相似结构的石墨相氮化碳(CN)表面, 同时构筑Fe₁单原子中心和临近的氮空位(N_V), 本工作设计制备了具有外围N_V修饰的Fe₁--N_V/CN单原子催化剂. 理论上, CN表面的N_V不仅能提升局部电子密度, 还可促进电子向邻近过渡金属位点的离域. 通过外围氮空位的调控策略, 本工作旨在优化Fe₁单原子位点的电子结构以提升其有氧氧化反应中的O₂活化性能. 基于球差电镜-扫描透射电镜、X-射线光电子能谱和X-射线吸收精细结构等表征技术, 揭示了催化剂中的Fe₁单原子位点的配位结构为Fe₁-N₅, 并且每个Fe₁-N₅位点锚定于CN载体表面的含有N_V的三-三嗪环结构单元上, 形成了长程的Fe₁--N_V双位点结构. 机理研究表明, Fe₁单原子位点可以优先吸附O₂分子, 而远程的N_V可以显著增强向Fe₁位点的电荷转移, 从而促使O₂快速转化为超氧自由基(·O₂⁻)和单线态氧(¹O₂)等活性物种. 得益于Fe₁--N_V双位点协同活化O₂过程, Fe₁--N_V/CN单原子催化剂在乙苯选择氧化至苯乙酮的反应中(120 ^oC, 6 bar O₂), TOF为373.4 h^-1, 选择性为~96.3%. 此外, 催化剂还具有优异的底物普适性.

本文通过精准构筑长程Fe₁--N_V双活性位点, 突破了传统单原子催化剂在电子转移效率方面的瓶颈, 为设计高效非贵金属催化剂提供了创新策略. 该仿生协同活化机制不仅深化了对催化氧化过程中O₂活化本质的理解, 更为开发绿色高效的工业催化体系开辟了新路径, 在精细化学品合成、污染物降解及清洁能源转化等领域展现出广阔应用前景.

关键词: 单原子催化剂, 外围氮物种影响, 长程氮空位, 协同催化, 有氧氧化

Abstract:

Catalytic oxidation plays a crucial role in chemical industry, in which the utilization of abundant and environmental-friendly oxygen (O₂) as oxidant aligns with sustainable development principles in green chemistry. However, the intrinsic inertness of ground-state O₂ molecule poses a long-standing challenge in developing an efficient non-noble metal-based catalyst. Herein, inspired by the electron transfer process in respiratory chain, we engineered long-range N_V to mediate Fe₁ center for O₂ activation in aerobic oxidation. Combined in/quasi-situ spectroscopic characterizations and control experiments suggest the Fe₁ site efficiently adsorbs O₂, and the N_V site facilitates electron delocalization to adjacent Fe₁, providing efficient transformation of O₂ to reactive oxygen species that boost oxidation reactions mildly. This Fe₁--N_V single-atom catalyst demonstrates outstanding catalytic performance in aerobic oxidations of alkanes, N-heterocycles, alcohols, and amines under relatively mild conditions. Our findings offer a new perspective for designing high-efficiency heterogeneous catalysts in aerobic oxidations, promising various potential applications.

Key words: Single-atom catalyst, Peripheral-nitrogen effect, Long-range N_V, Synergistic catalysis, Aerobic oxidation

刘粉利, 杨曼, 段江林, 殷祉钰, 史名扬, 陈馥清, 熊惠峰, 刘忻, 刘文刚, 夏琦兴, 孙少东, 冯丹, 齐海峰, 覃勇, 任煜京. 外围氮空位诱导电子传递至Fe单原子以实现高效的氧气活化过程[J]. 催化学报, 2025, 72: 187-198.

Fenli Liu, Man Yang, Jianglin Duan, Zhiyu Yin, Mingyang Shi, Fuqing Chen, Huifeng Xiong, Xin Liu, Wengang Liu, Qixing Xia, Shaodong Sun, Dan Feng, Haifeng Qi, Yong Qin, Yujing Ren. Peripheral N_V-induced electron transfer to Fe₁ single atoms for highly efficient O₂ activation[J]. Chinese Journal of Catalysis, 2025, 72: 187-198.

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https://www.cjcatal.com/CN/Y2025/V72/I5/187

图/表 6

Fig. 1. Schematic diagram of flavin-dependent monooxygenase and Fe1--NV/CN single-atom catalyst for the transformation of O2 into ROS. (a) The NAD(P)H and reduced flavin with nitrogen-containing heterocycles serve as the excited electron supplier in O2 to ROS transformation on Fe1-N4-S1 active center. (b) The nitrogen vacancy on carbon nitride surface facilitates the electron delocalization to adjacent Fe1 single-atom site for O2 activation.

Fig. 2. Schematic illustration of catalyst preparation and characterizations for Fe1--NV/CN catalyst. (a) Schematic illustration for Fe1--NV/CN catalyst synthesis. (b) N2 adsorption-desorption isotherms on Fe1--NV/CN. (c) XRD pattern of Fe1--NV/CN and CN samples. SEM image (scale bar = 3 μm) (d), HAADF-STEM (scale bar = 200 nm) (e), EDS-mapping images (scale bar = 200 nm) (f), and AC-HAADF-STEM (scale bar = 2 nm) image (g) of Fe1--NV/CN catalyst.

Fig. 3. Structural characterization of Fe1--NV/CN catalyst. N 1s XPS spectra (a), ratio of different N species to C (b), and ESR spectra (c) for CN and Fe1--NV/CN samples. Fe K-edge XANES (d) and FT-EXAFS (e) spectra of Fe1--NV/CN and Fe1/CN samples. The intensities of Fe Foil, FeO and Fe2O3 references are respectively multiplied by 1/15, 1/2 and 1/5. WT-EXAFS spectra (f) and EXAFS fitting curve (g) of Fe1--NV/CN and Fe1/CN samples. (h) The structural illustration of Fe1--NV sites on CN surface.

Fig. 4. Catalytic aerobic oxidation of ethylbenzene on Fe1--NV/CN catalyst. (a) Catalytic performance of CN, Fe1--NV/CN and Fe1/CN samples in aerobic oxidation of ethylbenzene. The apparent activation energy of Fe1--NV/CN (b) and Fe1/CN (c). (d) The catalytic activity comparison between Fe1--NV/CN and reported metal-based catalysts in aerobic oxidation of ethylbenzene. (e) The catalytic stability test of Fe1--NV/CN.

Fig. 5. Substrate scope of catalytic aerobic oxidations on Fe1--NV/CN catalyst. (a) Oxidative dehydrogenation of heterocycles on Fe1--NV/CN catalyst. (b) Selective oxidation of amines towards imine synthesis on Fe1--NV/CN catalyst. (c) Selective oxidation of alcohol to aldehyde on Fe1--NV/CN catalyst. (d) Selective oxidative of C-H bond towards ketones synthesis on Fe1--NV/CN catalyst. Reaction conditions: a 0.5 mmol substrate, 20 mg catalyst, 2 mL H2O, 10 bar air, 100 °C, isolated yield; b 120 °C. c 0.5 mmol substrate, 20 mg catalyst, 2 mL toluene, 30 bar air, 100 °C, 24 h, GC yield; d 1 mL substrate, 50 mg catalyst, 40 bar air, 120 °C, GC yield; 60 bar air, 150 °C.

Fig. 6. In-situ spectral characterization of O2 activation on Fe1--NV/CN and Fe1/CN catalysts. The quasi-situ XANES (a) and FT-EXAFS (b) spectra of Fe1--NV/CN and Fe1/CN catalysts with the sequential introduction of O2 and ethylbenzene (the intensity of Fe Foil is multiplied by 1/8). (c) The quasi-situ 57Fe M?ssbauer spectrum of Fe1--NV/CN catalyst with the introduction of O2. (d) The ESR spectra of Fe1--NV/CN and Fe1/CN with the addition of O2.

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外围氮空位诱导电子传递至Fe单原子以实现高效的氧气活化过程

Peripheral N_V-induced electron transfer to Fe₁ single atoms for highly efficient O₂ activation

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外围氮空位诱导电子传递至Fe单原子以实现高效的氧气活化过程

Peripheral NV-induced electron transfer to Fe1 single atoms for highly efficient O2 activation

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Peripheral N_V-induced electron transfer to Fe₁ single atoms for highly efficient O₂ activation