含双价态铂位点的Pt1/FeOx单原子催化剂用于水促进的硝基芳烃加氢反应

doi:10.1016/S1872-2067(26)65240-0

催化学报 ›› 2027, Vol. 92: 410-419.DOI: 10.1016/S1872-2067(26)65240-0

含双价态铂位点的Pt₁/FeO_x单原子催化剂用于水促进的硝基芳烃加氢反应

李安琦^a^,^b, 陈裕森^a^,^b, 潘晓丽^a, 任煜京^c, 曹宏晨^a^,^b, 毕桂月^a, 杨小峰^a^,^*(), 王爱琴^a^,^*(), 张涛^a^,^b^,^*()

^a 中国科学院大连化学物理研究所, 能源催化转化重点实验室, 辽宁大连 116023
^b 中国科学院大学, 北京 100049
^c 西北工业大学生命科学与技术学院, 生物与催化交叉研究中心, 陕西西安 710072

收稿日期:2026-07-06 接受日期:2026-08-19 出版日期:2027-01-02 发布日期:2026-10-30
通讯作者: *电子信箱: yangxf2003@dicp.ac.cn (杨小峰),
aqwang@dicp.ac.cn (王爱琴),
taozhang@dicp.ac.cn (张涛).
基金资助:
国家重点研发计划(2023YFA1506803);国家自然科学基金(22209171);国家自然科学基金(22132006);国家自然科学基金(22108259);国家自然科学基金委单原子催化研究中心(22388102)

Pt₁/FeO_x single-atom catalyst with dual-valent Pt sites for water-promoted hydrogenation of nitroarenes

Anqi Li^a^,^b, Yusen Chen^a^,^b, Xiaoli Pan^a, Yujing Ren^c, Hongchen Cao^a^,^b, Guiyue Bi^a, Xiaofeng Yang^a^,^*(), Aiqin Wang^a^,^*(), Tao Zhang^a^,^b^,^*()

^a State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
^b University of Chinese Academy of Sciences, Beijing 100049, China
^c Interdisciplinary Research Center of Biology and Catalysis, School of Life Science and Technology, Northwestern Polytechnical University, Xi’an 710072, Shaanxi, China

Received:2026-07-06 Accepted:2026-08-19 Online:2027-01-02 Published:2026-10-30
Contact: *E-mail: yangxf2003@dicp.ac.cn (X. Yang),
aqwang@dicp.ac.cn (A. Wang),
taozhang@dicp.ac.cn (T. Zhang).
Supported by:
National Key R&D Program of China(2023YFA1506803);National Natural Science Foundation of China(22209171);National Natural Science Foundation of China(22132006);National Natural Science Foundation of China(22108259);NSFC Center for Single-Atom Catalysis(22388102)

摘要/Abstract

摘要：

催化选择加氢在精细化学品、药品及农用化学品的合成中起着关键作用. 传统负载型金属纳米催化剂虽具有较高的加氢活性, 但在多官能团底物的选择性还原中, 往往面临化学选择性难以调控的难题. 在此背景下, 单原子催化剂（SACs）凭借其独特的空间构型与电子效应, 展现出官能团选择性活化与加氢的特殊潜力. 然而, 孤立单原子位点通常具有的阳离子特性限制其活化氢气的能力, 进而影响其催化加氢活性. 因此, 阐明不同价态单原子活性位的催化加氢性质及发展提升氢气活化效率的策略, 已成为选择加氢领域的共性挑战.

本文采用原子层沉积法将铂负载于α-Fe₂O₃纳米片, 成功合成了Pt₁/FeO_x单原子催化剂. 结构表征发现催化剂中存在Pt₁^δ⁺和Pt₁⁰两种价态不同的铂单原子活性位点, 且以Pt₁^δ⁺活性位占比为主导(76%). 密度泛函理论计算结果表明, 氢气在两种铂位点上具有显著不同的活化路径: 在Pt₁^δ⁺位点发生异裂活化, 而在Pt₁⁰位点则通过能垒较低的均裂机制活化, 且Pt₁⁰位点对H₂的活化活性显著高于Pt₁^δ⁺位点. 同时, 水分子介导的氢键网络可显著降低催化剂表面H₂解离及氢物种的溢流能垒, 而载体表面低价铁位点对硝基基团具有优异的活化能力. 宏观动力学分析、H₂-D₂和H₂-D₂O同位素交换及控制实验证实了水分子不仅促进且参与氢气活化, 并通过质子传递使得吸附于载体表面低价铁位点的硝基基团得以高效加氢. 3-硝基苯乙烯选择性加氢实验结果显示, 该双价态Pt₁/FeO_x单原子催化剂在反应中表现出优异的催化性能: 在含水量为50 vol%的溶剂中, 其周转频率约为纯乙醇体系中的24倍, 且目标产物3-氨基苯乙烯的选择性高达97.9%.

综上, 本文阐明了不同价态铂单原子的氢气活化机制, 揭示了水分子在单原子催化体系中的调控作用, 并明确了载体低价铁位点在硝基加氢反应中的活化机制, 从而在显著提升催化活性的同时保持了优异的加氢选择性. 该研究为高性能选择性加氢单原子催化剂的设计与开发提供了新思路.

关键词: 硝基芳烃加氢, 单原子催化剂, 水效应, 氢键网络, 选择性加氢

Abstract:

Single-atom catalysts (SACs) are highly attractive for selective hydrogenation owing to their excellent chemoselectivity toward specific functional group activation, yet the inherently cationic nature of isolated metal sites often limits hydrogen activation and thus compromises activity. Herein, we report a Pt₁/FeO_x SAC prepared via atomic layer deposition of Pt onto α-Fe₂O₃ nanosheets. Dual-valent Pt atoms are identified on different surface terminations of the exposed (001) facet, and theoretically demonstrated to exhibit distinct catalytic behaviors, i.e., Pt₁^δ⁺ sites enable heterolytic H₂ activation whereas Pt₁⁰ sites facilitate a more kinetically favorable homolytic H₂ dissociation. Moreover, a water-mediated hydrogen-bonding network substantially lowers the H₂ dissociation and H* species spillover barriers and promotes remote hydrogenation. As a result, in the catalytic hydrogenation of 3-nitrostyrene, the Pt₁/FeO_x SAC exhibits approximately 24-fold higher activity relative to its water-free counterpart, while high selectivity toward 3-aminostyrene is maintained through preferential activation of nitro groups at adjacent low-valence Fe neighboring Pt single-atom sites. These findings reveal that the catalytic behavior of SACs strongly depends on the oxidation state of single atoms. Notably, metallic single-atom species with water-promoted hydrogen activation demonstrate superior hydrogenation efficiency, resulting in a markedly enhanced activity.

Key words: Nitroarene hydrogenation, Single-atom catalysts, Water effect, Hydrogen-bonding network, Selective hydrogenation

李安琦, 陈裕森, 潘晓丽, 任煜京, 曹宏晨, 毕桂月, 杨小峰, 王爱琴, 张涛. 含双价态铂位点的Pt₁/FeO_x单原子催化剂用于水促进的硝基芳烃加氢反应[J]. 催化学报, 2027, 92: 410-419.

Anqi Li, Yusen Chen, Xiaoli Pan, Yujing Ren, Hongchen Cao, Guiyue Bi, Xiaofeng Yang, Aiqin Wang, Tao Zhang. Pt₁/FeO_x single-atom catalyst with dual-valent Pt sites for water-promoted hydrogenation of nitroarenes[J]. Chinese Journal of Catalysis, 2027, 92: 410-419.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65240-0

https://www.cjcatal.com/CN/Y2027/V92/I1/410

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Fig. 1. (a) H2-TPR profiles of Fe2O3 nanosheet and Pt/Fe2O3 catalyst. (b) HAADF-STEM image, (c) CO-DRIFTS and (d) in-situ XPS of Pt1/FeOx.

Fig. 2. (a) Top and side views of the geometry and charge density difference for the two Pt1/FeOx(001) models. The values for the calculated bader charges on the Pt1 are indicated. Charge accumulation and depletion are colored yellow and cyan, respectively, with the isosurface value of 0.01 e Å‒3. (b) The potential energy profiles for H2 dissociation and H species diffusion process on the two Pt1/FeOx(001) models. (c) PDOS of Pt atoms in the two Pt1/FeOx(001) models, the zero-energy corresponds to the Fermi level, and the d-band centers are shown with the dotted short lines. (d,e) The adsorption energies of H2, ‒NO2 and ‒C=C‒ group of 3-nitrostyrene on the different sites of Pt1/FeOx(001).

Fig. 3. (a) The energy barrier for H2 dissociation and H* spillover over the Pt1δ+/FeOx and Pt10/FeOx models, respectively, in the absence and presence of water. (b) The energy barrier for H* species diffusion over the O/Fe-terminated FeOx models in the absence and presence of water, respectively. (c,d) The potential energy profiles and schematic model for the H* species transferring from Pt1δ+ sites to the ‒NO2 group in the presence and absence of water. Color code: O-red; Fe-purple; Pt-blue; H-white; C-grey; N-dark blue.

Fig. 4. (a) Hydrogenation performance of 3-nitrostyrene as a function of added water content. 0.55 mmol 3-nitrostyrene, 40 mg Pt1/FeOx as catalyst, 100 μL n-octanol as internal standard, (x) mL H2O + (2‒x) mL ethanol as solvent in total. Reaction conditions: 40 °C, 0.4 MPa H2. 50 vol% water, x = 1 mL. The 3-nitrostyrene hydrogenation apparent activation energy (b), reaction order of 3-nitrostyrene (c) and H2 (d). (e) Kinetic isotope effect of H2/D2 and H2O/D2O in the hydrogenation of 3-nitrostyrene over Pt1/FeOx in ethanol or a mixture of ethanol and water (50 vol%). (f) H2-D2O isotopic exchange experiment results over Pt1/FeOx at 100 °C.

Fig. 5. (a) The mixing experiment of catalyst and WO3. Reaction conditions: 10 mg catalyst, 100 mg WO3, 2 mL solvent in total (2 mL ethanol or 1 mL ethanol + 1 mL water), 40 °C, 0.4 MPa H2, 20 min. (b) 3-Nitrostyrene hydrogenation performance over physical mixtures of PtNP/Al2O3 with Al2O3 or Fe2O3-S-230H2. Reaction conditions: 0.55 mmol 3-nitrostyrene, 30 mg PtNP/Al2O3 mixed with 30 mg support as catalyst, 100 μL n-octanol as internal standard, 2 mL ethanol or 1 mL ethanol + 1 mL water as solvent; 40 °C, 0.4 MPa H2.

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含双价态铂位点的Pt₁/FeO_x单原子催化剂用于水促进的硝基芳烃加氢反应

Pt₁/FeO_x single-atom catalyst with dual-valent Pt sites for water-promoted hydrogenation of nitroarenes

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