具有交错p-n异质结的光增强型Co单原子分散催化剂: 揭示其在锌-空气电池和燃料电池中的优异双功能性能

doi:10.1016/S1872-2067(25)64704-8

催化学报 ›› 2025, Vol. 73: 311-321.DOI: 10.1016/S1872-2067(25)64704-8

具有交错p-n异质结的光增强型Co单原子分散催化剂: 揭示其在锌-空气电池和燃料电池中的优异双功能性能

王昭娣^a, 张杨^a, 张军选^c, 徐能能^a(), 芦拓^a, 庄碧艳^a, 刘桂成^d(), 梁宇喆^c(), 雷浩^e, 田丙伦^e, 乔锦丽^a^,^b()

^a东华大学环境科学与工程学院, 先进纤维材料全国重点实验室, 上海 201620, 中国
^b上海市污染控制与生态安全研究所, 上海 200092, 中国
^c东国大学物理学院, 首尔, 韩国
^d华北电力大学新型储能技术北京实验室, 能源动力与机械工程学院, 北京 102206, 中国
^e协氢(上海)新能源科技有限公司, 上海 200333, 中国

收稿日期:2025-02-20 接受日期:2025-04-08 出版日期:2025-06-18 发布日期:2025-06-12
通讯作者: *电子信箱: nengnengxu@dhu.edu.cn (徐能能),gcliu@ncepu.edu.cn (刘桂成),wyang@dongguk.edu (梁宇喆),qiaojl@dhu.edu.cn (乔锦丽).
基金资助:
国家重点研发计划(2022YFE0138900);国家自然科学基金(21972017);上海市科委“科技创新行动计划”基础研究领域(19JC1410500);上海扬帆计划(22YF1400700);上海市教育发展基金会;上海市教育委员会晨光计划(22CGA37)

Photo-enhanced Co single-atom catalyst with a staggered p-n heterojunction: unraveling its high oxygen catalytic performance in zinc-air batteries and fuel cells

Zhaodi Wang^a, Yang Zhang^a, Junxuan Zhang^c, Nengneng Xu^a(), Tuo Lu^a, Biyan Zhuang^a, Guicheng Liu^d(), Woochul Yang^c(), Hao Lei^e, Binglun Tian^e, Jinli Qiao^a^,^b()

^aState Key Laboratory of Advanced Fiber Materials, College of Environmental Science and Engineering, Donghua University, Shanghai 201620, China
^bShanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China
^cDepartment of Physics, Dongguk University, Seoul 04620, Republic of Korea
^dBeijing Laboratory of New Energy Storage Technology, School of Energy Power and Mechanical Engineering, North China Electric Power University, Beijing 102206, China
^eHiTS (Shanghai) Hydrogen Power Technology Co., Ltd, Shanghai 200333, China

Received:2025-02-20 Accepted:2025-04-08 Online:2025-06-18 Published:2025-06-12
Contact: *E-mail: nengnengxu@dhu.edu.cn (N. Xu),gcliu@ncepu.edu.cn (G. Liu),wyang@dongguk.edu (W. Yang),qiaojl@dhu.edu.cn (J. Qiao).
Supported by:
National Key Research and Development Program of China(2022YFE0138900);National Natural Science Foundation of China(21972017);“Scientific and Technical Innovation Action Plan” Basic Research Field of Shanghai Science and Technology Committee(19JC1410500);Shanghai Sailing Program(22YF1400700);Chenguang Program of Shanghai Education the Development Foundation;Shanghai Municipal Education Commission(22CGA37)

摘要/Abstract

摘要：

随着化石燃料的枯竭和环境污染日益严重, 开发清洁高效的能源存储与转换技术迫在眉睫. 在众多候选技术中, 可充电的锌空气电池(ZABs)因其高理论能量密度(1084 Wh kg^-1)、低成本及环境友好特性备受关注, 被认为是大规模储能的重要候选技术. 质子交换膜燃料电池(PEMFCs)凭借高效、零排放的优势, 在能源转换领域也展现出巨大潜力. 然而, ZABs和PEMFCs的发展均受到氧还原反应(ORR)和析氧反应(OER)缓慢动力学的限制, 其关键瓶颈在于目前依赖的Pt基催化剂不仅成本高昂, 而且存在耐久性不足的问题. 光增强双功能催化剂通过利用光能降低反应过电位, 为突破这一瓶颈提供了新思路. 本研究通过构建g-C₃N₄@Co-N/MPC异质结催化剂, 不仅克服了传统催化剂的活性与稳定性方面的局限, 还为光电协同催化机制提供了新的解决方案, 对推动可再生能源技术的发展具有重要意义.

本文创新性地采用高能球磨法将g-C₃N₄与Co-N掺杂分级多孔碳(Co-N/MPC)复合, 构建了具有p-n异质结结构的光增强型双功能催化剂. 通过原子级分散的Co-N_x活性位点与p-n异质结的协同作用, 实现了以下突破: (1) Co-N/MPC载体具有超过800 m² g^-1的比表面积和分级孔道结构, 显著提升了活性位点密度和物质传质效率; (2) g-C₃N₄的引入不仅有效抑制Co原子的团聚, 并与Co-N/MPC形成的异质结更通过内置电场促进了光生载流子的分离, 使ORR/OER过电位差(ΔE)降至0.8864 V. 该催化剂直接作为空气电极应用于ZABs和H₂-空气燃料电池中, 可分别实现850.7和411 mW cm^-2的峰值功率密度功率, 并在250 h循环后仍保持优异稳定性. 机理研究表明, 性能提升归因于Co-N₄位点的高本征活性、分级孔道对传质的优化以及异质结界面上的内置电场对电荷分离的促进作用.

综上, 本工作为设计高效稳定的光-电协同催化剂提供了新策略, 通过原子级活性位点设计与异质结工程的结合, 不仅解决了传统催化剂的活性与稳定性难题, 更为开发高性能光增强型能量存储和转换体系开创新的路径.

关键词: 单原子Co, 分级多孔碳, 光增强, p-n异质结, 氧催化反应

Abstract:

The sluggish kinetics of the oxygen reduction reaction (ORR) and high over potential of oxygen evolution reaction (OER) are big challenges in the development of high-performance zinc-air batteries (ZABs) and fuel cells. In this work, we report a rational design and a simple fabrication strategy of a photo-enhanced Co single-atom catalyst (SAC) comprising g-C₃N₄ coupled with cobalt-nitrogen-doped hierarchical mesoporous carbon (Co-N/MPC), forming a staggered p-n heterojunction that effectively improves charge separation and enhances electrocatalytic activity. The incorporation of Co SACs and g-C₃N₄ synergistically optimizes the photogenerated electron-hole pair separation, significantly boosting the intrinsic ORR-OER duplex activity. Under illumination, g-C₃N₄@Co-N/MPC exhibits an outstanding ORR half-wave potential (E_1/2) of 0.841 V (vs. RHE) in 0.1 mol L^-1 KOH and a low OER overpotential of 497.4 mV (vs. RHE) at 10 mA cm^-2 in 1 mol L^-1 KOH. Notably, the catalyst achieves an exceptional peak power density of 850.7 mW cm^-2 in ZABs and of 411 mW cm^-2 even in H₂-air fuel cell. In addition, g-C₃N₄@Co-N/MPC-based ZABs also show remarkable cycling stability exceeding 250 h. The advanced photo-induced charge separation at the p-n heterojunction facilitates faster electron transfer kinetics, and the mass transport owing to hierarchical mesoporous structure of Co-N-C, thereby reducing the overpotential and enhancing the overall energy conversion efficiency. This work provides a new perspective on designing next-generation of single-atom dispersed oxygen reaction catalysts, paving the way for high-performance photo-enhanced energy storage and conversion systems.

Key words: Co single-atom, Hierarchical mesoporous carbon, Photo-enhancement, p-n Heterojunction, Oxygen catalytic reaction

王昭娣, 张杨, 张军选, 徐能能, 芦拓, 庄碧艳, 刘桂成, 梁宇喆, 雷浩, 田丙伦, 乔锦丽. 具有交错p-n异质结的光增强型Co单原子分散催化剂: 揭示其在锌-空气电池和燃料电池中的优异双功能性能[J]. 催化学报, 2025, 73: 311-321.

Zhaodi Wang, Yang Zhang, Junxuan Zhang, Nengneng Xu, Tuo Lu, Biyan Zhuang, Guicheng Liu, Woochul Yang, Hao Lei, Binglun Tian, Jinli Qiao. Photo-enhanced Co single-atom catalyst with a staggered p-n heterojunction: unraveling its high oxygen catalytic performance in zinc-air batteries and fuel cells[J]. Chinese Journal of Catalysis, 2025, 73: 311-321.

×
扫码分享

导出引用管理器 EndNote|Ris|BibTeX

链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(25)64704-8

https://www.cjcatal.com/CN/Y2025/V73/I6/311

图/表 5

Fig. 1. (a) Schematic diagram of the synthesis procedure of g-C3N4@Co-N/MPC. (b) SEM images of Co-N/MPC. (c) HAADF-STEM image of g-C3N4@Co-N/MPC. (d) Elemental mapping images. (e,f) TEM images of g-C3N4@Co-N/MPC.

Fig. 2. Physical characterization of Co-N/MPC and g-C3N4@Co-N/MPC. (a) XRD pattern for Co-N/MPC and g-C3N4@Co-N/MPC. (b) Raman spectrum. XPS spectra of C 1s (c) and N 1s (d). (e) A comparison chart illustrating the nitrogen content across various types. (f) Co K-edge XANES spectra of g-C3N4@Co-N/MPC with reference spectra of Co foil, CoO and CoPc. (g) The Fourier transform of the Co K-edge EXAFS spectra for the g-C3N4@Co-N/MPC with reference spectra of Co foil, CoO and CoPc. (h) The WT spectra of Co K edge EXAFS for Co foil, CoO, CoPc and g-C3N4@Co-N/MPC.

Fig. 3. (a) The ORR LSV polarization curves of g-C3N4, Co-N/MPC and g-C3N4@Co-N/MPC in O2-saturated 0.1 mol L-1 KOH electrolyte solution (1600 rpm) under light and darkness. (b) Comparison of E1/2 and limit current density. (c) The corresponding Tafel slopes. (d) Percentages of H2O2 produced and the electron transfer numbers of g-C3N4@Co-N/MPC under light and darkness. (e) The OER LSV polarization curves of g-C3N4, Co-N/MPC and g-C3N4@Co-N/MPC in 1 mol L-1 KOH electrolyte solution (1600 rpm) under light and darkness. (f) The corresponding Tafel slopes. (g) Comparison of bifunctional OER and ORR activity of g-C3N4@Co-N/MPC with other catalysts. (h) Comparison of ΔE. (i) Double-layer capacity of g-C3N4@Co-N/MPC under light and darkness.

Fig. 4. (a-c) Mott-Schottky plot of g-C3N4 (a), Co-N/MPC (b) and g-C3N4@Co-N/MPC (c). (d) UV-vis spectra. (e) Tauc plots. (f) Band structure diagram of g-C3N4@Co-N/MPC.

Fig. 5. Testing a complete zinc-air battery with photocatalyst g-C3N4@Co-N/MPC under light and darkness. (a) Schematic diagram of a zinc air battery. (b) OCV curves. (c) Discharge polarization curve and the corresponding power density curve. (d) Specific capacity plot. (e) The rate discharge test. (f) Comparison of zinc-air battery performance with various catalysts. (g) Polarization voltage curves for charging and discharging at 10 mA cm-2 constant currents. (h) Discharge polarization curves and the corresponding power density curves of a fuel cell under illumination and darkness.

参考文献

[1]	G. Nazir, A. Rehman, J. H. Lee, C. H. Kim, J. Gautam, K. Heo, S. Hussain, M. Ikram, A. A. AlObaid, S.-Y. Lee, S.-J. Park, Nano-Micro Lett., 2024, 16, 138.
[2]	S. Chen, H. Ren, Y. Qiu, C. Luo, Q. Zhao, W. Yang, J. Power Sources, 2023, 573, 233116.
[3]	A. S. Jamadar, R. Sutar, S. Patil, R. Khandekar, J. B. Yadav, Mater. Rep. Energy, 2024, 4, 100283.
[4]	L. Qiao, X. Wang, R. Xu, C. Zhang, K. Chen, K. Tong, H. Wang, S. Dai, L. Chu, M. Huang, Mater. Today Energy, 2023, 37, 101398.
[5]	J. Li, H. Xue, N. Xu, X. Zhang, Y. Wang, R. He, H. Huang, J. Qiao, Mater. Rep. Energy, 2022, 2, 100090.
[6]	W. Y. Wong, M. A. A. Abdul Rani, K. S. Loh, K. L. Lim, L. J. Minggu, Curr. Opin. Green Sustain. Chem., 2025, 52, 101001.
[7]	P. Phogat, B. Chand, Shreya, R. Jha, S. Singh, Int. J. Hydrogen Energy, 2025, 109, 465-485.
[8]	Y. Wang, S. Qin, F. Ma, C. Wang, W. He, B. Zhang, H. Li, Renewable Energy, 2025, 246, 122885.
[9]	X. Wang, L. Peng, N. Xu, M. Wu, Y. Wang, J. Guo, S. Sun, J. Qiao, ACS Appl. Mater. Interfaces, 2020, 12, 52836-52844.
[10]	S. Pan, Z. Ma, W. Yang, B. Dongyang, H. Yang, S. Lai, F. Dong, X. Yang, Z. Lin, Mater. Rep. Energy, 2023, 3, 100212.
[11]	X. Tang, F. Li, F. Li, Y. Jiang, C. Yu, Chin. J. Catal., 2023, 52, 79-98.
[12]	D. Du, S. Zhao, Z. Zhu, F. Li, J. Chen, Angew. Chem. Int. Ed., 2020, 59, 18140-18144.
[13]	Z. Jiang, Z. Li, Q. He, S. Han, Y. Liu, H. Zhu, X. Yuan, Mater. Rep. Energy, 2024, 4, 100267.
[14]	Y. Zhang, N. Xu, B. Gong, X. Ye, Y. Yang, Z. Wang, B. Zhuang, M. Wang, W. Yang, G. Liu, J. K. Lee, J. Qiao, Chin. J. Catal., 2025, 68, 300-310.
[15]	L. Hu, Y. Zhang, Q. Lin, F. Cao, W. Mo, S. Zhong, H. Lin, L. Xie, L. Zhao, S. Bai, Chin. J. Catal., 2025, 68, 311-325.
[16]	X. Lu, P. Yang, Y. Wan, H. Zhang, H. Xu, L. Xiao, R. Li, Y. Li, J. Zhang, M. An, Coord. Chem. Rev., 2023, 495, 215400.
[17]	C. Ye, L. Zhang, Y. Shen, ACS Mater. Lett., 2024, 6, 2858-2887.
[18]	K. Liu, J. Fu, Y. Lin, T. Luo, G. Ni, H. Li, Z. Lin, M. Liu, Nat. Commun., 2022, 13, 2075.
[19]	M. Zhang, H. Li, J. Chen, F.-X. Ma, L. Zhen, Z. Wen, C.-Y. Xu, Small, 2022, 18, 2202476.
[20]	S. Liang, L. C. Zou, L. J. Zheng, F. Li, X. X. Wang, L. N. Song, J. J. Xu, Adv. Energy Mater., 2022, 12, 2103097.
[21]	L. Zhao, Z. Zhang, Z. Zhu, P. Li, J. Jiang, T. Yang, P. Xiong, X. An, X. Niu, X. Qi, J.-S. Chen, R. Wu, Chin. J. Catal., 2023, 51, 216-224.
[22]	H. Gao, K. Liu, T. Luo, Y. Chen, J. Hu, J. Fu, M. Liu, Chin. J. Catal., 2022, 43, 832-838.
[23]	N. Song, J. Jiang, S. Hong, Y. Wang, C. Li, H. Dong, Chin. J. Catal., 2024, 59, 38-81.
[24]	F. Dong, C. Liu, M. Wu, J. Guo, K. Li, J. Qiao, ACS Sustainable Chem. Eng., 2019, 7, 8587-8596.
[25]	X. Dong, X. Luo, X. Yang, M. Wang, W. Xiao, Y. Liu, N. Xu, W. Yang, G. Liu, J. Qiao, J. Colloid Interface Sci., 2024, 672, 32-42.
[26]	P. Jiang, Y. Wang, Y. Li, L. Dai, N. Xu, J. Qiao, D. Ruan, Sep. Purif. Technol., 2024, 341, 126813.
[27]	Y. Wang, B. Yu, K. Liu, X. Yang, M. Liu, T.-S. Chan, X. Qiu, J. Li, W. Li, J. Mater. Chem. A, 2020, 8, 2131-2139.
[28]	M. Zhang, H. Li, J. Chen, F. X. Ma, L. Zhen, Z. Wen, C. Y. Xu, Adv. Funct. Mater., 2023, 33, 2370280.
[29]	J. Zhu, L. Huang, F. Bao, G. Chen, K. Song, Z. Wang, H. Xia, J. Gao, Y. Song, C. Zhu, F. Lu, T. Zheng, M. Ji, Mater. Rep. Energy, 2024, 4, 100245.
[30]	B. Zhou, N. Xu, L. Wu, D. Cai, E. H. Yu, J. Qiao, Green Energy Environ., 2024, 9, 1835-1846.
[31]	T. Lu, N. Xu, L. Guo, B. Zhou, L. Dai, W. Yang, G. Liu, J. K. Lee, J. Qiao, Adv. Fiber Mater., 2024, 6, 1108-1121.
[32]	J. Wang, W. H. Xuan, Q. He, J. X. Jiang, Y. Y. Zhou, Y. Nie, Q. Liao, M. H. Shao, W. Ding, Z. D. Wei, J. Electrochem., 2023, 29, 2215003.
[33]	X. Luo, Z. Zheng, B. Hou, X. Xie, C. C. Wang, RSC Adv., 2023, 13, 18888-18897.
[34]	K. Fu, Y. Wang, L. Mao, X. Yang, J. Jin, S. Yang, G. Li, Chem. Eng. J., 2018, 351, 94-102.
[35]	W.-F. Wu, J.-G. Fan, Z.-H. Zhao, J.-M. Pan, J. Yang, X. Yan, Y. Zhan, Chin. J. Catal., 2024, 60, 178-189.
[36]	S. Hu, P. Qiao, X. Liang, G. Ba, X. Zu, H. Hu, J. Ye, D. Wang, Appl. Catal. B, 2024, 346, 123737.
[37]	X. Zhou, D. Xu, J. Huang, S. Tong, P. Qiao, Z. Zhang, Adv. Funct. Mater., 2024, 2418055, 1-8.
[38]	J. E. Park, M. J. Kim, M. S. Lim, S. Y. Kang, J. K. Kim, S. H. Oh, M. Her, Y. H. Cho, Y. E. Sung, Appl. Catal. B, 2018, 237, 140-148.
[39]	J. Tian, Q. Liu, A. M. Asiri, K. A. Alamry, X. Sun, ChemSusChem, 2014, 7, 2125-2130.
[40]	Z. G. Liu, J. Zhao, H. Yao, X. X. He, H. Zhang, Y. Qiao, X. Q. Wu, L. Li, S. L. Chou, Chem. Sci., 2024, 15, 8478-8487.
[41]	T. Wu, M. Y. Han, Z. J. Xu, ACS Nano, 2022, 16, 8531-8539.
[42]	K. Xiao, X. Jiang, S. Zeng, J. Chen, T. Hu, K. Yuan, Y. Chen, Adv. Funct. Mater., 2024, 34, 2405830.
[43]	G. Gan, S. Fan, X. Li, J. Wang, C. Bai, X. Guo, M. Tade, S. Liu, ACS Catal., 2021, 11, 14284-14292.
[44]	J. X. Flores-Lasluisa, D. Cazorla-Amorós, E. Morallón, Nanomaterials, 2024, 14, 1381.
[45]	T. H. Nguyen, P. K. L. Tran, D. T. Tran, T. N. Pham, N. H. Kim, J. H. Lee, Chem. Eng. J., 2022, 440, 135781.
[46]	S. Biniak, G. Szymański, J. Siedlewski, A. Świątkowski, Carbon, 1997, 35, 1799-1810.
[47]	C. Y. Li, R. Zhang, X. J. Ba, X. L.Jiang, Y. Y. Yang, J. Electrochem., 2023, 29, 2210241.
[48]	Y. Zhu, Z. Zhang, Z. Lei, Y. Tan, W. Wu, S. Mu, N. Cheng, Carbon, 2020, 167, 188-195.
[49]	F. Wang, Y. Zhou, S. Lin, L. Yang, Z. Hu, D. Xie, Nano Energy, 2020, 78, 105128.
[50]	X. Li, F. Dong, N. Xu, T. Zhang, K. Li, J. Qiao, ACS Appl. Mater. Interfaces, 2018, 10, 15591-15601.
[51]	J. Shi, M. Fan, J. Qiao, Y. Liu, Chem. Lett., 2014, 43, 1484-1486.
[52]	B. Ravel, M. Newville, J. Synchrotron Radiat., 2005, 12, 537-541.
[53]	S. I. Zabinsky, J. J. Rehr, A. Ankudinov, R. C. Albers, M. J. Eller, Phys. Rev. B, 1995, 52, 2995-3009.
[54]	H. Funke, A. C. Scheinost, M. Chukalina, Phys. Rev. B, 2005, 71, 094110.
[55]	Z. Li, F. Liu, C. Chen, Y. Jiang, P. Ni, N. Song, Y. Hu, S. Xi, M. Liang, Y. Lu, Nano Lett., 2023, 23, 1505-1513.
[56]	V. Reisecker, F. Flatscher, L. Porz, C. Fincher, J. Todt, I. Hanghofer, V. Hennige, M. Linares-Moreau, P. Falcaro, S. Ganschow, S. Wenner, Y.-M. Chiang, J. Keckes, J. Fleig, D. Rettenwander, Nat. Commun., 2023, 14, 2432.
[57]	S.-Y. Ham, H. Yang, O. Nunez-cuacuas, D. H. S. Tan, Y.-T. Chen, G. Deysher, A. Cronk, P. Ridley, J.-M. Doux, E. A. Wu, J. Jang, Y. S. Meng, Energy Storage Mater., 2023, 55, 455-462.
[58]	Y. Chen, R. Ren, Z. Wen, S. Ci, J. Chang, S. Mao, J. Chen, Nano Energy, 2018, 47, 66-73.
[59]	A. Hankin, J. C. Alexander, G. H. Kelsall, Phys. Chem. Chem. Phys., 2014, 16, 16176-16186.
[60]	S. Harrison, M. Hayne, Sci. Rep., 2017, 7, 11638.
[61]	S. Fu, C. Peng, Y. Luo, L. Cheng, X. Yang, Z. Jiao, J. Colloid Interface Sci., 2024, 664, 349-359.
[62]	Z. Zhong, P. Hansmann, Phys. Rev. X, 2017, 7, 011023.
[63]	L. Tian, X. Guan, Y. Dong, S. Zong, A. Dai, Z. Zhang, L. Guo, Environ. Chem. Lett., 2023, 21, 1257-1264.
[64]	R. Ren, G. Liu, J. Y. Kim, R. E. A. Ardhi, M. X. Tran, W. Yang, J. K. Lee, Appl. Catal. B, 2022, 306, 121096.
[65]	Y. Ren, D. Zeng, W. J. Ong, Chin. J. Catal., 2019, 40, 289-319.
[66]	H. Li, B. Sun, F. Yang, Z. Wang, Y. Xu, G. Tian, K. Pan, B. Jiang, W. Zhou, RSC Adv., 2019, 9, 7870-7877.
[67]	Z. Yin, R. He, H. Xue, J. Chen, Y. Wang, X. Ye, N. Xu, J. Qiao, H. Huang, Energy Mater., 2022, 2, 200021.

具有交错p-n异质结的光增强型Co单原子分散催化剂: 揭示其在锌-空气电池和燃料电池中的优异双功能性能

Photo-enhanced Co single-atom catalyst with a staggered p-n heterojunction: unraveling its high oxygen catalytic performance in zinc-air batteries and fuel cells

RichHTML

PDF

Supporting Information

可视化

摘要/Abstract

引用本文

使用本文

扫码分享

图/表 5

参考文献

相关文章 2

编辑推荐

Metrics

[1]	吴春红, 方艳芬, Araya Hailu Tirusew, 向淼淼, 黄应平, 陈春城. p-n型异质结催化剂Ag₂O-BiVO₄对微囊藻毒素(MC-RR)的光化学氧化机理研究[J]. 催化学报, 2017, 38(2): 192-198.
[2]	法文君, 王平, 岳冰, 杨风岭, 李大鹏, 郑直. Ag₃PO₄/Ag₂CO₃p-n异质结复合光催化剂的制备及增强的可见光催化性能[J]. 催化学报, 2015, 36(12): 2186-2193.