基于氮杂Mn咔咯二维纳米材料的单原子Mn中心催化氧化烷烃制醇

doi:10.1016/S1872-2067(20)63707-X

催化学报 ›› 2021, Vol. 42 ›› Issue (6): 1030-1039.DOI: 10.1016/S1872-2067(20)63707-X

基于氮杂Mn咔咯二维纳米材料的单原子Mn中心催化氧化烷烃制醇

朱纯^a, 梁锦霞^b, 孟洋^a, 林坚^c^,^*(), 曹泽星^d^,^#()

^a贵州大学化学与化工学院, 贵州贵阳550025
^b贵州师范学院贵州省纳米材料模拟与计算重点实验室, 贵州贵阳550018
^c中国科学院大连化学物理研究所, 中国科学院航天催化材料重点实验室, 辽宁大连116023
^d厦门大学化学化工学院, 福建省理论与计算化学重点实验室, 福建厦门360015

收稿日期:2020-07-06 接受日期:2020-08-25 出版日期:2021-06-18 发布日期:2021-01-30
通讯作者: 林坚,曹泽星
基金资助:
国家自然科学基金(21663008);国家自然科学基金(21763006);国家自然科学基金(2193309);国家自然科学基金(21963005);国家自然科学基金(21878283);国家自然科学基金(22022814);贵州省自然科学基金([2017]1029);中国科学院青年创新促进会(2017223)

Mn-corrolazine-based 2D-nanocatalytic material with single Mn atoms for catalytic oxidation of alkane to alcohol

Chun Zhu^a, Jin-Xia Liang^b, Yang Meng^a, Jian Lin^c^,^*(), Zexing Cao^d^,^#()

^aSchool of Chemistry and Chemical Engineering, Guizhou University, Guiyang 550025, Guizhou, China
^bGuizhou Provincial Key Laboratory of Computational Nano-Material Science, Guizhou Education University, Guiyang 550018, Guizhou, China
^cCAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
^dState Key Laboratory of Physical Chemistry of Solid Surfaces and Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 360015, Fujian, China

Received:2020-07-06 Accepted:2020-08-25 Online:2021-06-18 Published:2021-01-30
Contact: Jian Lin,Zexing Cao
About author:^#Tel: +86-592-2186081; Fax: +86-592-2183047; E-mail: zxcao@xmu.edu.cn
^*Tel: +86-411-84379673; Fax: +86-411-84685940; E-mail: jianlin@dicp.ac.cn;
Supported by:
National Natural Science Foundation of China(21663008);National Natural Science Foundation of China(21763006);National Natural Science Foundation of China(2193309);National Natural Science Foundation of China(21963005);National Natural Science Foundation of China(21878283);National Natural Science Foundation of China(22022814);Natural Science Foundation of Guizhou Province of China([2017]1029);Youth Innovation Promotion Association CAS(2017223)

摘要/Abstract

摘要：

咔咯是由四个吡咯共轭相连而形成的具有芳香性的新型卟啉类大环化合物, 但咔咯分子中存在一个直接连结两个吡咯环的C-C键, 与卟啉相比, 仅仅是少了一个“meso”位置的C原子. 因此, 在结构上, 咔咯含有三个“吡咯型”氮原子和一个“吡啶型”氮原子, 当咔咯失去三个内氢原子后变成了三价阴离子, 易与金属形成高价态的稳定配合物. 氮杂咔咯是一种咔咯的meso位上的C被取代为N的咔咯衍生物. 与正常的咔咯相比, 它更易于与过渡金属形成稳定配合物. 正是由于这些独特的结构特点, 使其在金属催化、染料敏化太阳能电池、光敏剂、金属传感器、甚至在医学上都有很好的应用前景.
金属有机大环均相催化剂的非均相化, 是改进反应产物分离和实现催化剂循环使用的最简单有效方法之一. 环境友好的Mn氮杂咔咯催化剂, 在温和条件下可以利用氧气直接将有机底物氧化. 本文选用Mn氮杂咔咯催化剂作为基本构建单元, 通过理论计算, 构建了一种新型的具有高催化活性的含Mn氮杂咔咯环结构单元的二维纳米催化材料. 我们分别使用高斯软件(Gaussian 09)和维也纳从头算模拟软件包(VASP)对孤立分子和周期性体系进行结构优化以及性质的计算. 在这种二维材料中, 每一个Mn原子作为相对独立的金属单原子中心(SAC), 保留了单环中Mn金属中心的高催化活性. 在温和的光照条件下, Mn金属中心可以直接活化氧气生成类自由基[Mn]-O-O中心, 随后[Mn]-O-O中心可以有效地通过夺取有机底物中的H和紧接着新生自由基的偶合反应, 选择性氧化C-H键为C-OH键. 另外, 通过沿[Mn]-O-O反应轴施加不同强度的外电场, 可对此二维纳米材料的催化反应活性进行精细调控. 本文为实验上制备基于Mn氮杂咔咯的非均相催化剂以及单原子Mn基催化剂提供了理论依据.

关键词: 单原子催化剂, 非均相化, 二维纳米材料, 第一性原理计算, C-H键的活化

Abstract:

Heterogenization of organic-macrocyclic metal catalysts is one of the simplest and most efficient methods for effective separation of products and cyclic application of a catalyst. By using an environmentally friendly Mn-corrolazine catalyst as the building unit, which can directly oxidize organic substrates under oxygen atmosphere and mild conditions, we theoretically constructed a novel two-dimensional (2D) Mn-corrolazine nanocatalytic material with high catalytic activity. In this material, each Mn atom maintains its electronic configuration in the monomer and can directly activate O₂ as the single-atom catalyst (SAC) center to form a radical-like [Mn]-O-O under mild visible-light irradiation conditions. The newly generated [Mn]-O-O can efficiently and selectively oxidize C-H bonds to form alcohol species through H-abstraction and the rebound reaction. Moreover, the catalytic reaction is easily regulated by an external electric field along its intrinsic Mn-O-O reaction axis. The current study provides a theoretical foundation for further experimental studies and practical applications of the Mn-corrolazine-based SAC.

Key words: Single-atom catalyst, Heterogenization, Two-dimensional nanomaterials, First-principles calculations, C-H bond activation

朱纯, 梁锦霞, 孟洋, 林坚, 曹泽星. 基于氮杂Mn咔咯二维纳米材料的单原子Mn中心催化氧化烷烃制醇[J]. 催化学报, 2021, 42(6): 1030-1039.

Chun Zhu, Jin-Xia Liang, Yang Meng, Jian Lin, Zexing Cao. Mn-corrolazine-based 2D-nanocatalytic material with single Mn atoms for catalytic oxidation of alkane to alcohol[J]. Chinese Journal of Catalysis, 2021, 42(6): 1030-1039.

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https://www.cjcatal.com/CN/Y2021/V42/I6/1030

图/表 11

Scheme 1. Manganese corrolazine dimer (di-Mncor), tetramer (tetra-Mncor) and their extended two-dimensional nanocatalytic material (2D-Mncor) constructed by combining Mn-corrolazines and ethynes.

Fig. 1. Optimized geometries and relatively energies (kcal/mol) of di-Mncor in (a) singlet and (b) nonet states; tetra-Mncor in (c) singlet and (d) 17-et states (top view).

Table 1 Selected optimized bond lengths (?), Mulliken spin densities (ρspin) of Mn, magnetic moment (μB), and relative energies (ΔE, kcal/mol) of Mn(III)-corrolazine in di-Mncor in the singlet and nonet states, tetra-Mncor in the single and 17-et states, 2D-Mncor with ferromagnetism (FM) and antiferromagnetism (AFM).

Polymer (State)	d_Mn-N1 d_Mn-N2	d_Mn-N3 d_Mn-N4	d_c≡c	ΔE	ρ_spin/μ_B Mn
Di-Mn_cor (nonet)	1.864, 1.864 1.864, 1.864	1.860, 1.861 1.860, 1.861	1.218, 1.218	0.0	3.77, 3.77
Di-Mn_cor (singlet)	1.848, 1.848 1.848, 1.848	1.863, 1.863 1.863, 1.862	1.218, 1.218	98.65	—
Tetra-Mn_cor (17-et)	1.865, 1.878 1.866, 1.879 1.866, 1.880 1.866, 1.878	1.868, 1.867 1.868, 1.867 1.868, 1.867 1.868, 1.866	1.215, 1.222 1.215, 1.223 1.216, 1.224 1.216, 1.224	0.0	3.77, 3.77 3.77, 3.77
Tetra-Mn_cor (singlet)	1.847, 1.856 1.847, 1.856 1.847, 1.856 1.848, 1.856	1.865, 1.865 1.865, 1.865 1.865, 1.865 1.865, 1.865	1.216, 1.222 1.216, 1.222 1.217, 1.224 1.217, 1.224	194.38	—
2D-Mn_cor (FM)	1.903, 1.904 1.903, 1.904	1.885, 1.886 1.885, 1.886	1.230, 1.231	13.34	3.57, 3.57
2D-Mn_cor (AFM)	1.903, 1.904 1.903, 1.905	1.885, 1.886 1.885, 1.887	1.231, 1.231	0.0	3.65, -3.65

Fig. 2. Selected Mn-dominated molecular orbitals of the di-Mncor in the nonet state.

Table 2 The bond lengths of Mn-N (?), the relative energies (ΔG, kcal/mol) and Mulliken spin densities (ρspin), selected atoms’ magnetic moments (μB) of the complexes of O2 and Mn(III)-corrolazine in different states of di-O-Mncor, tetra-O-Mncor and 2D-Mncor.

Polymer (State)	d_Mn-N1 d_Mn-N2	d_Mn-N3 d_Mn-N4	d_O-O	ΔE	ρ_spin/μ_B
Polymer (State)	d_Mn-N1 d_Mn-N2	d_Mn-N3 d_Mn-N4	d_O-O	ΔE	^aO	^bO	Mn
Di-O-Mn_cor (13-et)	1.867, 1.868 1.867, 1.868	1.865, 1.864 1.864, 1.864	1.214 1.214	0.0	1.03 1.03	0.98 0.98	3.77 3.77
Di-O-Mn_cor (quintet)	1.874, 1.874 1.874, 1.873	1.871, 1.871 1.871, 1.871	1.216 1.216	2.98	-1.03 -1.03	-0.92 -0.92	3.74 3.74
Di-O-Mn_cor (singlet)	1.871, 1.877 1.873, 1.876	1.899, 1.894 1.896, 1.894	1.256 1.256	84.14	—	—	—
Tetra-O-Mn_cor (singlet)	1.858, 1.897 1.865, 1.894 1.858, 1.897 1.865, 1.894	1.886, 1.894 1.893, 1.898 1.886, 1.894 1.893, 1.898	1.254 1.255 1.255 1.256	—	—	—	—
2D-O-Mn_cor (spin-polarized)	1.921, 1.923 1.920, 1.921	1.903, 1.902 1.903, 1.904	1.262 1.262	0.0	-0.73 0.73	-0.58 0.57	3.58 -3.58
2D-O-Mn_cor (spin-unpolarized)	1.925, 1.929 1.927, 1.928	1.917, 1.918 1.917, 1.918	1.267 1.267	74.53	—	—	—

Fig. 3. Optimized geometries of di-O-Mncor complexes consisting of O2 and di-Mncor in (a) singlet, (b) quintet, and (c) 13-et states. (d) Tetra-O-Mncor in the singlet state consisting of O2 and tetra-Mncor with specific bond lengths (?).

Fig. 4. The optimized structures of quintet-, triplet- and singlet-state complexes of Mn(III)-corrolazine and 3[O2] and the energy difference between corresponding two complexes with different spin multiplicities.

Fig. 5. (a) Optimized geometry and (b) the electronic band structure of 2D-Mncor nanomaterial

Fig. 6. The predicted reaction pathway for the generation of cyclohexanol and the Mn(V)-oxo unit catalyzed by the 2D-O-Mncor nanomaterial in the spin-unpolarized state (relative energies and selected bond lengths are in kcal/mol and ?, respectively).

Fig. 7. Proposed reaction pathway for CH4 activation on the 2D-O-Mncor nanomaterial in the spin-unpolarized state (relative energies and selected bond lengths are in kcal/mol and ?, respectively).

Fig. 8. Predicted barriers for the conversion of CH4 to CH3OH under various external electric fields.

参考文献

[1]	J. F. B. Barata, M. G. P. M. S. Neves, M. A. F. Faustino, A. C. Tomé, J. A. S. Cavaleiro, Chem. Rev., 2017,117, 3192-3253.
[2]	A. Ghosh, Chem. Rev., 2017,117, 3798-3881.
[3]	C. Zhu, J. Liang, B. Wang, J. Zhu, Z. Cao, Phys. Chem. Chem. Phys., 2012,14, 12800-12806.
[4]	P. Li, Z. Cao, Organometallics, 2018,37, 406-414.
[5]	Z. Gross, N. Galili, I. Saltsman, Angew. Chem. Int. Ed., 1999,38, 1427-1429.
[6]	I. Aviv-Harel, Z. Gross, Coord. Chem. Rev., 2011,255, 717-736.
[7]	H.-Y. Liu, M. H. R. Mahmood, S.-X. Qiu, C. K. Chang, Coord. Chem. Rev., 2013,257, 1306-1333.
[8]	A. Mahammed, Z. Gross, Coord. Chem. Rev., 2019,379, 121-132.
[9]	S. Nardis, F. Mandoj, M. Stefanelli, R. Paolesse, Coord. Chem. Rev., 2019,388, 360-405.
[10]	W. Liu, X. Huang, M.-J. Cheng, R. J. Nielsen, W. A. Goddard, J. T. Groves, Science, 2012,337, 1322-1325.
[11]	S. Leininger, B. Olenyuk, P. J. Stang, Chem. Rev., 2000,100, 853-908.
[12]	W. Nam, Acc. Chem. Res., 2007,40, 522-531.
[13]	G. Golubkov, J. Bendix, H. B. Gray, A. Mahammed, I. Goldberg, A. J. DiBilio, Z. Gross, Angew. Chem. Int. Ed., 2001,40, 2132-2134.
[14]	N. Wang, H. Zheng, W. Zhang, R. Cao, Chin. J. Catal., 2018,39, 228-244.
[15]	E. Vogel, S. Will, A. S. Tilling, L. Neumann, J. Lex, E. Bill, A. X. Trautwein, K. Wieghardt, Angew. Chem. Int. Ed., 1994,33, 731-735.
[16]	A. E. Meier-Callahan, H. B. Gray, Z. Gross, Inorg. Chem., 2000,39, 3605-3607.
[17]	G. Golubkov, Z. Gross, Angew. Chem. Int. Ed., 2003,42, 4507-4510.
[18]	C. Zhu, J.-X. Liang, J. Power Sources, 2015,283, 343-350.
[19]	C. Zhu, J. Liang, Z. Cao, J. Phys. Chem. C, 2013,117, 13388-13395.
[20]	C. Brückner, C. A. Barta, R. P. Briñas, J. A. K. Bauer, Inorg. Chem., 2003,42, 1673-1680.
[21]	I. Aviv, Z. Gross, Chem. Commun., 2007, 1987-1999.
[22]	P. Li, Z. Cao, Dalton Trans., 2019,48, 1344-1350.
[23]	K. A. Prokop, D. P. Goldberg, J. Am. Chem. Soc., 2012,134, 8014-8017.
[24]	C. Zhu, J.-X. Liang, Z. Cao, J. Phys. Chem. C, 2018,122, 20781-20786.
[25]	J. P. T. Zaragoza, T. H. Yosca, M. A. Siegler, P. Moënne-Loccoz, M. T. Green, D. P. Goldberg, J. Am. Chem. Soc., 2017,139, 13640-13643.
[26]	X. He, Q. He, Y. Deng, M. Peng, H. Chen, Y. Zhang, S. Yao, M. Zhang, D. Xiao, D. Ma, B. Ge, H. Ji, Nat. Commun., 2019,10, 3663.
[27]	T. Stergiannakos, E. Tylianakis, E. Klontzas, P. N. Trikalitis, G. E. Froudakis, J. Phys. Chem. C, 2012,116, 8359-8363.
[28]	Y. Wang, W. Zhang, D. Deng, X. Bao, Chin. J. Catal., 2017,38, 1443-1453.
[29]	M.-J. Sun, X. Cao, Z. Cao, Nanoscale, 2018,10, 10450-10458.
[30]	L. Wu, X. Cao, W. Hu, Y. Ji, Z.-Z. Zhu, X.-F. Li, ACS Appl. Energy Mater., 2019,2, 6634-6641.
[31]	J.-X. Liang, J. Lin, J. Liu, X. Wang, T. Zhang, J. Li, Angew. Chem. Int. Ed., 2020,59, 12868-12875.
[32]	A. Wang, J. Li, T. Zhang, Nat. Rev. Chem., 2018,2, 65-81.
[33]	B. Qiao, A. Wang, X. Yang, L. F. Allard, Z. Jiang, Y. Cui, J. Liu, J. Li, T. Zhang, Nat. Chem., 2011,3, 634-641.
[34]	Y. Pan, Y. Chen, K. Wu, Z. Chen, S. Liu, X. Cao, W.-C. Cheong, T. Meng, J. Luo, L. Zheng, C. Liu, D. Wang, Q. Peng, J. Li, C. Chen, Nat. Commun., 2019,10, 4290.
[35]	K. Jiang, S. Back, A. J. Akey, C. Xia, Y. Hu, W. Liang, D. Schaak, E. Stavitski, J. K. Nørskov, S. Siahrostami, H. Wang, Nat. Commun., 2019,10, 3997.
[36]	M. Flytzani-Stephanopoulos, Chin. J. Catal., 2017,38, 1432-1442.
[37]	K. Liu, X. Zhao, G. Ren, T. Yang, Y. Ren, A. F. Lee, Y. Su, X. Pan, J. Zhang, Z. Chen, J. Yang, X. Liu, T. Zhou, W. Xi, J. Luo, C. Zeng, H. Matsumoto, W. Liu, Q. Jiang, K. Wilson, A. Wang, B. Qiao, W. Li, T. Zhang, Nat. Commun., 2020,11, 1263.
[38]	J. Liang, X. Yang, C. Xu, T. Zhang, J. Li, Chin. J. Catal., 2017,38, 1566-1573.
[39]	Y. Ren, Y. Tang, L. Zhang, X. Liu, L. Li, S. Miao, D. Sheng Su, A. Wang, J. Li, T. Zhang, Nat. Commun., 2019,10, 4500.
[40]	B. Qiao, J.-X. Liang, A. Wang, J. Liu, T. Zhang, Chin. J. Catal., 2016,37, 1580-1586.
[41]	Y. Tang, C. Asokan, M. Xu, G. W. Graham, X. Pan, P. Christopher, J. Li, P. Sautet, Nat. Commun., 2019,10, 4488.
[42]	F. Chen, X. Jiang, L. Zhang, R. Lang, B. Qiao, Chin. J. Catal., 2018,39, 893-898.
[43]	T. Yang, R. Fukuda, S. Hosokawa, T. Tanaka, S. Sakaki, M. Ehara, ChemCatChem, 2017,9, 1222-1229.
[44]	M. Zhou, M. Yang, X. Yang, X. Zhao, L. Sun, W. Deng, A. Wang, J. Li, T. Zhang, Chin. J. Catal., 2020,41, 524-532.
[45]	Y.-G. Wang, D. Mei, V.-A. Glezakou, J. Li, R. Rousseau, Nat. Commun., 2015,6, 6511.
[46]	Y. Tang, Y.-G. Wang, J.-X. Liang, J. Li, Chin. J. Catal., 2017,38, 1558-1565.
[47]	B. Qiao, J. Lin, A. Wang, Y. Chen, T. Zhang, J. Liu, Chin. J. Catal., 2015,36, 1505-1511.
[48]	Q. Shang, N. Tang, H. Qi, S. Chen, G. Xu, C. Wu, X. Pan, X. Wang, Y. Cong, Chin. J. Catal., 2020,41, 1812-1817.
[49]	J. Liang, Q. Yu, X. Yang, T. Zhang, J. Li, Nano Res., 2018,11, 1599-1611.
[50]	R. Shediac, M. H. B. Gray, H. T. Uyeda, R. C. Johnson, J. T. Hupp, P. J. Angiolillo, M. J. Therien, J. Am. Chem. Soc., 2000,122, 7017-7033.
[51]	M. J. Frisch, G. W. Trucks, H. B. Schlegel, G. E. Scuseria, M. A. Robb, J. R. Cheeseman, G. Scalmani, V. Barone, B. Mennucci, G. A. Petersson, H. Nakatsuji, M. Caricato, X. Li, H. P. Hratchian, A. F. Izmaylov, J. Bloino, G. Zheng, J. L. Sonnenberg, M. Hada, M. Ehara, K. Toyota, R. Fukuda, J. Hasegawa, M. Ishida, T. Nakajima, Y. Honda, O. Kitao, H. Nakai, T. Vreven, J. A. Jr., Montgomery, J. E. Peralta, F. Ogliaro, M. Bearpark, J. J. Heyd, E. Brothers, K. N. Kudin, V. N. Staroverov, R. Kobayashi, J. Normand, K. Raghavachari, A. Rendell, J. C. Burant, S. S. Iyengar, J. Tomasi, M. Cossi, N. Rega, N. J. Millam, M. Klene, J. E. Knox, J. B. Cross, V. Bakken, C. Adamo, J. Jaramillo, R. Gomperts, R. E. Stratmann, O. Yazyev, A. J. Austin, R. Cammi, C. Pomelli, J. W. Ochterski, R. L. Martin, K. Morokuma, V. G. Zakrzewski, G. A. Voth, P. Salvador, J. J. Dannenberg, S. Dapprich, A. D. Daniels, Ö. Farkas, J. B. Foresman, J. V. Ortiz, J. Cioslowski, D. J. Fox, Gaussian 09, Revision B.01, Gaussian, Inc., Wallingford CT, 2009.
[52]	C. Lee, W. Yang, R. G. Parr, Phys. Rev. B, 1988,37, 785-789.
[53]	A. D. Becke, J. Chem. Phys., 1993,98, 5648-5652.
[54]	G. Kresse, J. Hafner, Phys. Rev. B, 1993,47, 558-561.
[55]	G. Kresse, D. Joubert, Phys. Rev. B, 1999,59, 1758-1775.
[56]	S. L. Dudarev, G. A. Botton, S. Y. Savrasov, C. J. Humphreys, A. P. Sutton, Phys. Rev. B, 1998,57, 1505-1509.
[57]	A. Wadehra, J. W. Nicklas, J. W. Wilkins, Appl. Phys. Lett., 2010,97, 092119.
[58]	P. Deák, B. Aradi, T. Frauenheim, E. Janzén, A. Gali, Phys. Rev. B, 2010,81, 153203.
[59]	J. X. Liang, S. B. Tang, Z. X. Cao, J. Phys. Chem. C, 2011,115, 18802-18809.
[60]	S. Grimme, J. Antony, S. Ehrlich, H. Krieg, J. Chem. Phys., 2010,132, 154104.
[61]	A. Kumar, I. Goldberg, M. Botoshansky, Y. Buchman, Z. Gross, J. Am. Chem. Soc., 2010,132, 15233-15245.
[62]	J.-X. Liang, C.-J. Zhang, Acta Chim. Sin., 2010,68, 7-12.
[63]	R. O. Jones, J. Chem. Phys., 1999,110, 5189-5200.
[64]	C. Zhang, W. Sun, Z. Cao, J. Am. Chem. Soc., 2008,130, 5638-5639.
[65]	N. Tsunoji, H. Nishida, Y. Ide, K. Komaguchi, S. Hayakawa, Y. Yagenji, M. Sadakane, T. Sano, ACS Catal., 2019,9, 5742-5751.
[66]	J. Li, Z. Zhang, L. Wu, W. Zhang, P. Chen, Z. Lin, G. Liu, Nature, 2019,574, 516-521.
[67]	V. Postils, M. Rodríguez, G. Sabenya, A. Conde, M. M. Díaz-Requejo, P. J. Pérez, M. Costas, M. Solà, J. M. Luis, ACS Catal., 2018,8, 4313-4322.
[68]	S. Shaik, D. Kumar, S. P. de Visser, A. Altun, W. Thiel, Chem. Rev., 2005,105, 2279-2328.
[69]	P. Schwach, X. Pan, X. Bao, Chem. Rev., 2017,117, 8497-8520.
[70]	N. J. Gunsalus, A. Koppaka, S. H. Park, S. M. Bischof, B. G. Hashiguchi, R. A. Periana, Chem. Rev., 2017,117, 8521-8573.
[71]	J. Lin, X. Wang, Sci. China Mater., 2018,61, 758-760.
[72]	Z. Wang, D. Danovich, R. Ramanan, S. Shaik, J. Am. Chem. Soc., 2018,140, 13350-13359.
[73]	J. Joy, T. Stuyver, S. Shaik, J. Am. Chem. Soc., 2020,142, 3836-3850.

基于氮杂Mn咔咯二维纳米材料的单原子Mn中心催化氧化烷烃制醇

Mn-corrolazine-based 2D-nanocatalytic material with single Mn atoms for catalytic oxidation of alkane to alcohol

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