非金属电催化剂环境条件下氮还原反应的研究进展

doi:10.3866/PKU.WHXB202009043

Abstract

Abstract:

NH₃ plays an important role in modern society as an essential building block in the manufacture of fertilizers, aqueous ammonia, plastics, explosives, and dyes. Additionally, it is regarded as a green alternative fuel, owing to its carbon-free nature, large hydrogen capacity, high energy density, and easy transportation. The Haber-Bosch process plays a dominant role in global NH₃ synthesis; however, it involves high pressure and temperature and employs N₂ and H₂ as feeding gases, thus suffering from high energy consumption and substantial CO₂ emission. As a promising alternative to the Haber-Bosch process, electrochemical N₂ reduction enables sustainable and environmentally benign NH₃ synthesis under ambient conditions. Moreover, its applied potential is compatible with intermittent solar, wind, and other renewable energies. However, efficient electrocatalysts are required to drive N₂-to-NH₃ conversion because of the extremely inert N≡N bond. To date, significant efforts have been made to explore high-performance catalysts with high efficiency and selectivity. Generally, noble-metal catalysts exhibit efficient performance for the NRR, but their scarcity and high cost limit their large-scale application. Therefore, considerable attention has been focused on earth-abundant transition-metal (TM) catalysts that can use empty or unoccupied orbitals to accept the lone-pair electrons of N₂, while donating the abundant d-orbital electrons to the antibonding orbitals of N₂. However, these catalysts may release metal ions, leading to environmental pollution. Most of these TM electrocatalysts may also favor the formation of TM—H bonds, facilitating the hydrogen evolution reaction (HER) during the electrocatalytic reaction. Recent years have seen a surge in the exploration of metal-free catalysts (MFCs). MFCs mainly include carbon-based catalysts (CBCs) and some boron-based and phosphorus-based catalysts. Generally, CBCs exhibit a porous structure and high surface area, which are favorable for exposing more active sites and providing rich accessible channels for mass/electron transfer. Moreover, the Lewis acid sites of most metal-free compounds could accept the lone-pair electron of N₂ and adsorb N₂ molecules by forming nonmetal—N bonds, further widening their potential for electrocatalytic NRR. Compared with metal-based catalysts, the occupied orbitals of metal-free catalysts can only form covalent bonds or conjugated π bonds, hindering electron donation from the electrocatalyst to N₂ and molecular activation. In this review, we summarize the recent progress in the design and development of metal-free electrocatalysts (MFCs) for the ambient NRR, including carbon-based catalysts, boron-based catalysts, and phosphorus-based catalysts. In particular, heteroatom doping (N, O, S, B, P, F, and co-dopants), organic polymers, carbon nitride, and defect engineering are highlighted. We also discuss strategies to boost NRR performance and provide an outlook on the development perspectives of MFCs.

Key words: Electrochemistry, Metal-free catalysts, Ambient condition, N₂ reduction reaction, NH₃ synthesis

Tong Xu, Benyuan Ma, Jie Liang, Luchao Yue, Qian Liu, Tingshuai Li, Haitao Zhao, Yonglan Luo, Siyu Lu, Xuping Sun. Recent Progress in Metal-Free Electrocatalysts toward Ambient N₂ Reduction Reaction[J]. Acta Phys. -Chim. Sin. 2021, 37(7), 2009043. doi: 10.3866/PKU.WHXB202009043

Figures/Tables 15

Catalyst	Electrolyte	Potential (V vs. RHE)	NH₃ yield	FE (%)	Reference
NPC-750	0.05 mol·L⁻¹ H₂SO₄	−0.9	1.4 mmol·h⁻¹·g⁻¹	1.42	47
C-ZIF	0.1 mol·L⁻¹ KOH	−0.3	3.4 × 10⁻⁶ mol·cm⁻²·h⁻¹	10.2	48
N-doped carbon nanospikes	0.25 mol·L⁻¹ LiClO₄	−1.19	97.18 μg·h⁻¹·cm⁻²	11.56	49
NCM	0.1 mol·L⁻¹ HCl	−0.3	0.08 g·m⁻²·h⁻¹	5.2	50
NC from bamboo shoots	0.1 mol·L⁻¹ HCl	−0.35	16.3 μg·h⁻¹·mg⁻¹	27.5	51
NCF from cicada	0.1 mol·L⁻¹ HCl	−0.2	15.7 μg·h⁻¹·mg⁻¹	1.45	54
NPGC from alfalfa	0.005 mol·L⁻¹ H₂SO₄	−0.4	1.31 mmol·h⁻¹·g⁻¹	9.98	52
O-doped graphene	0.1 mol·L⁻¹ HCl	−0.55	21.3 μg·h⁻¹·mg⁻¹	12.6	55
O-KFCNTs from kapok fibers	0.1 mol·L⁻¹ HCl	−0.85	25.12 μg·h⁻¹·mg⁻¹	9.1	39
O-CNs from tannin	0.1 mol·L⁻¹ HCl	−0.6	20.15 μg·h⁻¹·mg⁻¹	4.97	46
O-doped porous carbon	0.1 mol·L⁻¹ HCl	−0.55	18.03 μg·h⁻¹·mg⁻¹	10.3	38
S-doped carbon nanosphere	0.1 mol·L⁻¹ Na₂SO₄	−0.7	19.07 μg·h⁻¹·mg⁻¹	7.47	57
Sulfur dots-graphene	0.5 mol·L⁻¹ LiClO₄	−0.85	28.56 μg·h⁻¹·mg⁻¹	7.07	60
S-doped 3D-graphene	0.05 mol·L⁻¹ H₂SO₄	−0.6	38.81 μg·h⁻¹·mg⁻¹	7.72	59
S-doped graphene	0.1 mol·L⁻¹ HCl	−0.6	27.3 μg·h⁻¹·mg⁻¹	11.5	58
B-doped graphene	0.05 mol·L⁻¹ H₂SO₄	−0.5	9.8 μg·h⁻¹·cm⁻²	10.8	64
P-doped graphene	0.5 mol·L⁻¹ LiClO₄	−0.65	32.33 μg·h⁻¹·mg⁻¹	20.82	66
Fluorographene nanosheet	0.1 mol·L⁻¹ Na₂SO₄	−0.7	9.3 μg·h⁻¹·mg⁻¹	4.2	69
F-doped 3D porous carbon framework	0.05 mol·L⁻¹ H₂SO₄	−0.2	197.7 μg·h⁻¹·mg⁻¹	54.8	70
B, N co-doped graphene	0.1 mol·L⁻¹ HCl	−0.3	7.75 μg·h⁻¹·mg⁻¹	13.79	73
B, N co-doped porous carbon nanofiber	0.1 mol·L⁻¹ KOH	−0.7	32.5 μg·h⁻¹·mg⁻¹	13.2	74
N, P co-doped porous carbon	0.1 mol·L⁻¹ HCl	−0.2	0.97 μg·h⁻¹·mg⁻¹	4.2	75
N, S co-doped graphene	0.1 mol·L⁻¹ HCl	−0.6	7.7 μg·h⁻¹·mg⁻¹	5.8	76
PANI/CP	0.1 mol·L⁻¹ HCl	−0.7	5.45 × 10⁻¹¹ mol·s⁻¹·cm⁻²	3.76	79
PTCA-rGO	0.1 mol·L⁻¹ HCl	−0.5	24.7 μg·h⁻¹·mg⁻¹	6.9	81
PEBCD/C	0.5 mol·L⁻¹ Li₂SO₄	−0.5	1.58 μg·h⁻¹·cm⁻²	2.85	84
PCN-NV4	0.1 mol·L⁻¹ HCl	−0.2	8.09 μg·h⁻¹·mg⁻¹	11.59	42
CC-450	0.1 mol·L⁻¹ Na₂SO₄	−0.3	2.59 × 10⁻¹⁰ mol·cm⁻²·s⁻¹	6.92	88
DG-800	0.01 mol·L⁻¹ H₂SO₄	−0.4	4.31 μg·h⁻¹·mg⁻¹	8.51	89
O-CNT	0.1 mol·L⁻¹ LiClO₄	−0.4	32.33 μg·h⁻¹·mg⁻¹	12.5	90
TA-rGO	0.5 mol·L⁻¹ LiClO₄	−0.75	17.02 μg·h⁻¹·mg⁻¹	4.83	91
2D boron nanosheets	0.1 mol·L⁻¹ Na₂SO₄	−0.8	13.22 μg·h⁻¹·mg⁻¹	4.04	97
B₄C nanosheets	0.1 mol·L⁻¹ HCl	−0.75	26.57μg·h⁻¹·mg⁻¹	15.95	6
h-BNNS	0.1 mol·L⁻¹ HCl	−0.75	22.4 μg·h⁻¹·mg⁻¹	4.7	104
FL-BP NSs	0.01 mol·L⁻¹ HCl	−0.7	33.37 μg·h⁻¹·mg⁻¹	5.07	107
BP nanoparticles	0.1 mol·L⁻¹ HCl	−0.6	26.42 μg·h⁻¹·mg⁻¹	12.7	115

References 115

1	Rosca V. ; Duca M. ; de Groot M. T. ; Koper M. T. M. Chem. Rev. 2009, 109, 2209. doi: 10.1021/cr8003696
2	Schlögl R. Angew. Chem. Int. Ed. 2003, 42, 2004. doi: 10.1002/anie.200301553
3	Klerke A. ; Christensen C. H. ; Nørskov J. K. ; Vegge T. J. Mater. Chem. 2008, 18, 2304. doi: 10.1039/b720020j
4	Dybkjaer, I. Ammonia Production Processes.In Ammonia, Catalysis and Manufacture; Nielsen, A., Ed.; Springer Publishing: Heidelberg, Germany, 1995; pp. 199−327.
5	Shipman M. A. ; Symes M. D. Catal. Today 2017, 286, 57. doi: 10.1016/j.cattod.2016.05.008
6	Qiu W. B. ; Xie X. Y. ; Qiu J. D. ; Fang W. H. ; Liang R. P. ; Ren X. ; Ji X. Q. ; Cui G. W. ; Asiri A. M. ; Cui G. L. ; et al Nat. Commun. 2018, 9, 3485. doi: 10.1038/s41467-018-05758-5
7	Zhu X. J. ; Mou S. Y. ; Peng Q. L. ; Liu Q. ; Luo Y. L. ; Chen G. ; Gao S. Y. ; Sun X. P. J. Mater. Chem. A. 2020, 8, 1545. doi: 10.1039/c9ta13044f
8	Lv X. ; Wang F. Y. ; Du J. ; Liu Q. ; Luo Y. S. ; Lu S. Y. ; Chen G. ; Gao S. Y. ; Zheng B. Z. ; Sun X. P. Sustain. Energy Fuels 2020, 4, 4469. doi: 10.1039/d0se00828a
9	Zhao R. B. ; Liu C. W. ; Zhang X. X. ; Zhu X. J. ; Wei P. P. ; Ji L. ; Guo Y. B. ; Gao S. Y. ; Luo Y. S. ; Wang Z. M. ; et al J. Mater. Chem. A 2020, 8, 77. doi: 10.1039/c9ta10346e
10	Bao D. ; Zhang Q. ; Meng F. L. ; Zhong H. X. ; Shi M. M. ; Zhang Y. ; Yan J. M. ; Jiang Q. ; Zhang X. B. Adv. Mater. 2017, 29, 1604799. doi: 10.1002/adma.201604799
11	Deng G. R. ; Wang T. ; Alshehri A. A. ; Alzahrani K. A. ; Wang Y. ; Ye H. J. ; Luo Y. L. ; Sun X. P. J. Mater. Chem. A 2019, 7, 21674. doi: 10.1039/c9ta06523g
12	Liu H. M. ; Han S. H. ; Zhao Y. ; Zhu Y. Y. ; Tian X. L. ; Zeng J. H. ; Jiang J. X. ; Xia B. Y. ; Chen Y. J. Mater. Chem. A 2018, 6, 3211. doi: 10.1039/c7ta10866d
13	Wang J. ; Liu Y. P. ; Zhang H. ; Huang D. J. ; Chu K. Catal. Sci. Technol. 2019, 9, 4248. doi: 10.1039/c9cy00907h
14	Yu J. L. ; Li C. B. ; Li B. Y. ; Zhu X. J. ; Zhang R. ; Ji L. ; Tang D. P. ; Asiri A. M. ; Sun X. P. ; Li Q. ; et al Chem. Commun. 2019, 55, 6401. doi: 10.1039/c9cc02310k
15	Li C. B. ; Ma D. W. ; Mou S. Y. ; Luo Y. S. ; Ma B. Y. ; Lu S. Y. ; Cui G. W. ; Li Q. ; Liu Q. ; Sun X. P. J. Energy Chem. 2020, 50, 402. doi: 10.1016/j.jechem.2020.03.044
16	Gao J. J. ; Lv X. ; Wang F. Y. ; Luo Y. S. ; Lu S. Y. ; Chen G. ; Gao S. Y. ; Zhong B. H. ; Guo X. D. ; Sun X. P. J. Mater. Chem. A 2020, 8, 17956. doi: 10.1039/d0ta07720h
17	Liu Q. ; Zhang X. X. ; Zhang B. ; Luo Y. L. ; Cui G. W. ; Xie F. Y. ; Sun X. P. Nanoscale 2018, 10, 14386. doi: 10.1039/c8nr04524k
18	Ren X. ; Zhao J. X. ; Wei Q. ; Ma Y. J. ; Guo H. R. ; Liu Q. ; Wang Y. ; Cui G. W. ; Asiri A. M. ; Li B. H. ; et al ACS Cent. Sci. 2019, 5, 116. doi: 10.1021/acscentsci.8b00734
19	Wang Y. ; Jia K. ; Pan Q. ; Xu Y. D. ; Liu Q. ; Cui G. W. ; Guo X. D. ; Sun X. P. ACS Sustain. Chem. Eng. 2019, 7, 117. doi: 10.1021/acssuschemeng.8b05332
20	Wei P. P. ; Xie H. T. ; Zhu X. J. ; Zhao R. B. ; Ji L. ; Tong X. ; Luo Y. S. ; Cui G. W. ; Wang Z. M. ; Sun X. P. ACS Sustain. Chem. Eng. 2020, 8, 29. doi: 10.1021/acssuschemeng.9b06272
21	Zhu X. J. ; Liu Z. C. ; Wang H. B. ; Zhao R. B. ; Chen H. Y. ; Wang T. ; Wang F. X. ; Luo Y. L. ; Wu Y. P. ; Sun X. P. Chem. Commun. 2019, 55, 3987. doi: 10.1039/c9cc00647h
22	Xiong W. ; Cheng X. ; Wang T. ; Luo Y. S. ; Feng J. ; Lu S. Y. ; Asiri A. M. ; Li W. ; Jiang Z. J. ; Sun X. P. Nano Res. 2020, 13, 1008. doi: 10.1007/s12274-020-2733-9
23	Liu Y. P. ; Li Y. B. ; Huang D. J. ; Zhang H. ; Chu K. Chem. Eur. J. 2019, 25, 11933. doi: 10.1002/chem.201902156
24	Cheng X. ; Wang J. W. ; Xiong W. ; Wang T. ; Wu T. W. ; Lu S. Y. ; Chen G. ; Gao S. Y. ; Shi X. F. ; Jiang Z J. ; et al ChemNanoMat 2020, 6, 1315. doi: 10.1002/cnma.202000110
25	Xu T. ; Ma D. W. ; Li C. B. ; Liu Q. ; Lu S. Y. ; Asiri A. M. ; Yang C. ; Sun X. P. Chem. Commun. 2020, 56, 3673. doi: 10.1039/c9cc10087c
26	Wu T. W. ; Zhao H. T. ; Zhu X. J. ; Xing Z. ; Liu Q. ; Liu T. ; Gao S. Y. ; Lu S. Y. ; Chen G. ; Asiri A M. ; et al Adv. Mater. 2020, 32, 2000299. doi: 10.1002/adma.202000299
27	Xia L. ; Li B. H. ; Zhang Y. ; Zhang R. ; Ji L. ; Chen H. Y. ; Cui G. W. ; Zheng H. G. ; Sun X. P. ; Xie F. Y. ; Liu Q. Inorg. Chem. 2019, 58, 2257. doi: 10.1021/acs.inorgchem.8b03143
28	Qin Q. ; Zhao Y. ; Schmallegger M. ; Heil T. ; Schmidt J. ; Walczak R. ; Gescheidt D. G. ; Jiao H. J. ; Oschatz M. Angew. Chem. Int. Ed. 2019, 58, 13101. doi: 10.1002/anie.201906056
29	Wu T. W. ; Kong W. H. ; Zhang Y. ; Xing Z. ; Zhao J. X. ; Wang T. ; Shi X. F. ; Luo Y. L. ; Sun X. P. Small Methods 2019, 3, 1900356. doi: 10.1002/smtd.201900356
30	Zhang X. X. ; Liu Q. ; Shi X. F. ; Asiri A. M. ; Luo Y. L. ; Sun X. P. ; Li T. S. J. Mater. Chem. A. 2018, 6, 17303. doi: 10.1039/c8ta05627g
31	Han J. R. ; Liu Z. C. ; Ma Y. J. ; Cui G. W. ; Xie F. Y. ; Wang F. X. ; Wu Y. P. ; Gao S. Y. ; Xu Y. H. ; Sun X. P. Nano Energy 2018, 52, 264. doi: 10.1016/j.nanoen.2018.07.045
32	Zhang Y. ; Qiu W. B. ; Ma Y. J. ; Luo Y. L. ; Tian Z. Q. ; Cui G. W. ; Xie F. Y. ; Chen L. ; Li T. S. ; Sun X. P. ACS Catal. 2018, 8, 8540. doi: 10.1021/acscatal.8b02311
33	Zhu X. J. ; Liu Z. C. ; Liu Q. ; Luo Y. L. ; Shi X. F. ; Asiri A. M. ; Wu Y. P. ; Sun X. P. Chem. Commun. 2018, 54, 11332. doi: 10.1039/c8cc06366d
34	Li Y. F. ; Li T. S. ; Zhu X. J. ; Alshehri A. A. ; Alzahrani K. A. ; Lu S. Y. ; Sun X. P. Chem. Asian J. 2020, 15, 487. doi: 10.1002/asia.201901624
35	Zhu X. J. ; Wu T. W. ; Ji L. ; Liu Q. ; Luo Y. L. ; Cui G. W. ; Xiang Y. M. ; Zhang Y. N. ; Zheng B. Z. ; Sun X. P. Chem. Commun. 2020, 56, 731. doi: 10.1039/c9cc08352a
36	Chen J. Y. ; Huang H. ; Xia L. ; Xie H. T. ; Ji L. ; Wei P. P. ; Zhao R. B. ; Chen H. Y. ; Asiri A. M. ; Sun X. P. ChemistrySelect 2019, 4, 3547. doi: 10.1002/slct.201900253
37	Wu T. T. ; Li P. P. ; Wang H. B. ; Zhao R. B. ; Li H. ; Kong W. H. ; Liu M. L. ; Zhang Y. Y. ; Sun X. P. ; Gong F. Chem. Commun. 2019, 55, 2684. doi: 10.1039/c8cc09867k
38	Zhao S. L. ; Lu X. Y. ; Wang L. Z. ; Gale J. ; Amal R. Adv. Mater. 2019, 31, 1805367. doi: 10.1002/adma.201805367
39	Zhang L. L. ; Chen G. F. ; Ding L. X. ; Wang H. H. Chem. Eur. J. 2019, 25, 12464. doi: 10.1002/chem.201901668
40	Lv C. D. ; Qian Y. M. ; Yan C. S. ; Ding Y. ; Liu Y. Y. ; Chen G. ; Yu G. H. Angew. Chem. Int. Ed. 2018, 57, 10246. doi: 10.1002/anie.201806386
41	Wan Y. C. ; Xu J. C. ; Lv R. T. Mater. Today 2019, 27, 69. doi: 10.1016/j.mattod.2019.03.002
42	Kitano M. ; Kanbara S. ; Inoue Y. ; Kuganathan N. ; Sushko P. V. ; Yokoyama T. ; Hara M. ; Hosono H. Nat. Commun. 2015, 6, 6731. doi: 10.1038/ncomms7731
43	Huang C. S. ; Li Y. J. ; Wang N. ; Xue Y. R. ; Zuo Z. C. ; Liu H. B. ; Li Y. L. Chem. Rev. 2018, 118, 7744. doi: 10.1021/acs.chemrev.8b00288
44	Liu Q. L. ; Wang S. N. ; Chen G. L. ; Liu Q. C. ; Kong X. K. Inorg. Chem. 2019, 58, 11843. doi: 10.1021/acs.inorgchem.9b02280
45	Huang H. ; Xia L. ; Cao R. R. ; Niu Z. G. ; Chen H. Y. ; Liu Q. ; Li T. S. ; Shi X. F. ; Asiri A. M. ; Sun X. P. Chem. Eur. J. 2019, 25, 1914. doi: 10.1002/chem.201805523
46	Ling C. Y. ; Bai X. W. ; Ouyang Y. X. ; Du A. J. ; Wang J. L. J. Phys. Chem. C 2018, 122, 16842. doi: 10.1021/acs.jpcc.8b05257
47	Liu Y. M. ; Su Y. ; Quan X. ; Fan X. F. ; Chen S. ; Yu H. T. ; Zhao H. M. ; Zhang Y. B. ; Zhao J. J. ACS Catal. 2018, 8, 1186. doi: 10.1021/acscatal.7b02165
48	Mukherjee S. ; Cullen D. A. ; Karakalos S. ; Liu K. X. ; Zhang H. ; Zhao S. ; Xu H. ; More K. L. ; Wang G. F. ; Wu G. Nano Energy 2018, 48, 217. doi: 10.1016/j.nanoen.2018.03.059
49	Song Y. ; Johnson D. ; Peng R. ; Hensley D. K. ; Bonnesen P. V. ; Liang L. B. ; Huang J. S. ; Yang F C. ; Zhang F. ; Qiao R. ; et al Sci. Adv. 2018, 4, e1700336. doi: 10.1126/sciadv.1700336
50	Wang H. ; Wang L. ; Wang Q. ; Ye S. Y. ; Sun W. ; Shao Y. ; Jiang Z. P. ; Qiao Q. ; Zhu Y. M. ; Song P F. ; et al Angew. Chem. Int. Ed. 2018, 57, 12360. doi: 10.1002/anie.201805514
51	Li Q. L. ; Chen X. F. ; Yang Y. Catalysts 2020, 10, 353. doi: 10.3390/catal10030353
52	Zhao C. J. ; Zhang S. B. ; Han M. M. ; Zhang X. ; Liu Y. Y. ; Li W. Y. ; Chen C. ; Wang G. Z. ; Zhang H. M. ; Zhao H. J. ACS Energy Lett. 2019, 4, 377. doi: 10.1021/acsenergylett.8b02138
53	Chen X. R. ; Guo Y. T. ; Du X. C. ; Zeng Y. S. ; Chu J. W. ; Gong C. H. ; Huang J. W. ; Fan C. ; Wang X. F. ; Xiong J. Adv. Energy Mater. 2020, 10, 1903172. doi: 10.1002/aenm.201903172
54	Yang X. X. ; Li K. ; Cheng D. M. ; Pang W. L. ; Lv J. Q. ; Chen X. Y. ; Zang H. Y. ; Wu X. L. ; Tan H. Q. ; Wang Y.H. ; et al J. Mater. Chem. A. 2018, 6, 7762. doi: 10.1039/c8ta01078a
55	Wang T. ; Xia L. ; Yang J. J. ; Wang H. B. ; Fang W. H. ; Chen H. Y. ; Tang D. P. ; Asiri A. M. ; Luo Y. L. ; Cui G L. ; et al Chem. Commun. 2019, 55, 7502. doi: 10.1039/c9cc01999e
56	Hoffman B. M. ; Lukoyanov D. ; Yang Z. Y. ; Dean D. R. ; Seefeldt L. C. Chem. Rev. 2014, 114, 4041. doi: 10.1021/cr400641x
57	Xia L. ; Wu X. F. ; Wang Y. ; Niu Z. G. ; Liu Q. ; Li T. S. ; Shi X. F. ; Asiri A. M. ; Sun X. P. Small Methods 2018, 3, 1800251. doi: 10.1002/smtd.201800251
58	Xia L. ; Yang J. J. ; Wang H. B. ; Zhao R. B. ; Chen H. Y. ; Fang W. H. ; Asiri A. M. ; Xie F. Y. ; Cui G. L. ; Sun X. P. Chem. Commun. 2019, 55, 3371. doi: 10.1039/c9cc00602h
59	Wang J. ; Wang S. ; Li J. P. Dalton Trans. 2020, 49, 2258. doi: 10.1039/c9dt04827h
60	Chen H. Y. ; Zhu X. J. ; Huang H. ; Wang H. B. ; Wang T. ; Zhao R. B. ; Zheng H. G. ; Asiri A. M. ; Luo Y. L. ; Sun X. P. Chem. Commun. 2019, 55, 3152. doi: 10.1039/c9cc00461k
61	Légaré M. A. ; Bélanger-Chabot G. ; Dewhurst R. D. ; Welz E. ; Krummenacher I. ; Engels B. ; Braunschweig H. Science 2018, 359, 896. doi: 10.1126/science.aaq1684
62	Hering-Junghans C. Angew. Chem. Int. Ed. 2018, 57, 6738. doi: 10.1002/anie.201802675
63	Liu C. W. ; Li Q. Y. ; Wu C. Z. ; Zhang J. ; Jin Y. G. ; MacFarlane D. R. ; Sun C. H. J. Am. Chem. Soc. 2019, 141, 2884. doi: 10.1021/jacs.8b13165
64	Yu X. M. ; Han P. ; Wei Z. X. ; Huang L. S. ; Gu Z. X. ; Peng S. J. ; Ma J. M. ; Zheng G. F. Joule 2018, 2, 1610. doi: 10.1016/j.joule.2018.06.007
65	Ling C. Y. ; Niu X. H. ; Li Q. ; Du A. J. ; Wang J. L. J. Am. Chem. Soc. 2018, 140, 14161. doi: 10.1021/jacs.8b07472
66	Wu T. W. ; Li X. Y. ; Zhu X. J. ; Mou S. Y. ; Luo Y. L. ; Shi X. F. ; Asiri A. M. ; Zhang Y. N. ; Zheng B. Z. ; Zhao H T. ; et al Chem. Commun. 2020, 56, 1831. doi: 10.1039/c9cc09179c
67	Inagaki M. ; Kang F. Y. J. Mater. Chem. A. 2014, 2, 13193. doi: 10.1039/c4ta01183j
68	Paupitz R. ; Autreto P. A. S. ; Legoas S. B. ; Srinivasan S. G. ; van Duin A. C. T. ; Galvão D. S. Nanotechnology 2012, 24, 035706. doi: 10.1088/0957-4484/24/3/035706
69	Zhao J. X. ; Yang J. J; Ji. ; L . ; Wang H. B. ; Chen H. Y. ; Niu Z. G. ; Liu Q. ; Li T. S. ; Cui G. W. ; Sun X. P. Chem. Commun. 2019, 55, 4266. doi: 10.1039/c9cc01920k
70	Liu Y. ; Li Q. Y. ; Guo X. ; Kong X. D. ; Ke J. W. ; Chi M. F. ; Li Q. X. ; Geng Z. G. ; Zeng J. Adv. Mater. 2020, 32, 1907690. doi: 10.1002/adma.201907690
71	Montoya J. H. ; Tsai C. ; Vojvodic A. ; Nørskov J. K. ChemSusChem 2015, 8, 2180. doi: 10.1002/cssc.201500322
72	Ling C. Y. ; Ouyang Y. X. ; Li Q. ; Bai X. W. ; Mao X. ; Du A. J. ; Wang J. L. Small Methods 2018, 1800376. doi: 10.1002/smtd.201800376
73	Chen C. ; Yan D. F. ; Wang Y. ; Zhou Y. Y. ; Zou Y. Q. ; Li Y. F. ; Wang S. Y. Small 2019, 15, 1805029. doi: 10.1002/smll.201805029
74	Kong Y. ; Li Y. ; Yang B. ; Li Z. J. ; Yao Y. ; Lu J. G. ; Lei L. C. ; Wen Z. H. ; Shao M. H. ; Hou Y. J. Mater. Chem. A 2019, 7, 26272. doi: 10.1039/c9ta06076f
75	Song P. F. ; Wang H. ; Kang L. ; Ran B. C. ; Song H. H. ; Wang R. M. Chem. Commun. 2019, 55, 687. doi: 10.1039/c8cc09256g
76	Tian Y. ; Xu D. Z. ; Chu K. ; Wei Z. ; Liu W. M. J. Mater. Sci. 2019, 54, 9088. doi: 10.1007/s10853-019-03538-0
77	Köleli F. ; Röpke T. Appl. Catal. B: Environ. 2006, 62, 306. doi: 10.1016/j.apcatb.2005.08.006
78	Köleli F. ; Kayan D. B. J. Electroanal. Chem. 2010, 638, 119. doi: 10.1016/j.jelechem.2009.10.010
79	Yu J. L. ; Li J. ; Zhu X. J. ; Zhang X. X. ; Jia K. ; Kong W. H. ; Wei P. P. ; Chen H. Y. ; Shi X. F. ; Asiri A. M. ; et al ChemElectroChem 2019, 6, 2215. doi: 10.1002/celc.201900320
80	Kumar C. V. S. ; Subramanian V. Phys. Chem. Chem. Phys. 2017, 19, 15377. doi: 10.1039/c7cp02220d
81	Li P. P. ; Wang J. W. ; Chen H. Y. ; Sun X. P. ; You J. M. ; Liu S. H. ; Zhang Y. Y. ; Liu M. L. ; Niu X. B. ; Luo Y. L. J. Mater. Chem. A 2019, 7, 12446. doi: 10.1039/c9ta03654g
82	Marcia M. ; Hirsch A. ; Hauke F. FlatChem 2017, 1, 89. doi: 10.1016/j.flatc.2017.01.001
83	Yuan Y. L. ; Gou X. X. ; Yuan R. ; Chai Y. Q. ; Zhuo Y. ; Ye X. Y. ; Gan X. X. Biosens. Bioelectron. 2011, 30, 123. doi: 10.1016/j.bios.2011.08.041
84	Chen G. F. ; Cao X. R. ; Wu S. Q. ; Zeng X. Y. ; Ding L. X. ; Zhu M. ; Wang H. H. J. Am. Chem. Soc. 2017, 139, 9771. doi: 10.1021/jacs.7b04393
85	Ji S. ; Wang Z. X. ; Zhao J. X. J. Mater. Chem. A 2019, 7, 2392. doi: 10.1039/c8ta10497b
86	Cao Y. Y. ; Deng S. W. ; Fang Q. J. ; Sun X. ; Zhao C. X. ; Zheng J. N. ; Gao Y. J. ; Zhuo H. ; Li Y. J. ; Yao Z H. ; et al Nanotechnol. 2019, 30, 335403. doi: 10.1088/1361-6528/ab1d01
87	Zhang J. ; Zhao Y. M. ; Wang Z. ; Yang G. ; Tian J. L. ; Ma D. W. ; Wang Y. X. New J. Chem. 2020, 44, 422. doi: 10.1039/c9nj04792a
88	Li W. Y. ; Wu T. X. ; Zhang S. B. ; Liu Y. Y. ; Zhao C. J. ; Liu G. Q. ; Wang G. Z. ; Zhang H. M. ; Zhao H. J. Chem. Commun. 2018, 54, 11188. doi: 10.1039/c8cc06000b
89	Du Y. Q. ; Jiang C. ; Xia W. ; Song L. ; Li P. ; Gao B. ; Wu C. ; Sheng L. ; Ye J H. ; Wang T. ; et al J. Mater. Chem. A 2020, 8, 55. doi: 10.1039/c9ta10071g
90	Zhao J. X. ; Wang B. ; Zhou Q. ; Wang H. B. ; Li X. H. ; Chen H. Y. ; Wei Q. ; Wu D. ; Luo Y. L. ; You J M. ; et al Chem. Commun. 2019, 55, 4997. doi: 10.1039/c9cc00726a
91	Song Y. Y. ; Wang T. ; Sun J. W. ; Wang Z. C. ; Luo Y. L. ; Zhang L. X. ; Ye H. J. ; Sun X. P. ACS Sustain. Chem. Eng. 2019, 7, 14368. doi: 10.1021/acssuschemeng.9b03890
92	Liu C. W. ; Li Q. Y. ; Zhang J. ; Jin Y. G. ; MacFarlane D. R. ; Sun C. H. J. Phys. Chem. C 2018, 122, 25268. doi: 10.1021/acs.jpcc.8b10021
93	Tang H. ; Ismail-Beigi S. Phys. Rev. Lett. 2007, 11, 115501. doi: 10.1103/physrevlett.99.115501
94	Szwacki G. N. ; Sadrzadeh A. ; Yakobson B. I. Phys. Rev. Lett. 2007, 16, 166804. doi: 10.1103/physrevlett.98.166804
95	Oganov A. R. ; Chen J. H. ; Gatti C. ; Ma Y. Z. ; Ma Y. M. ; Glass C. W. ; Liu Z. X. ; Yu T. ; Kurakevych O. O. ; Solozhenko V. L. Nature 2009, 460, 292. doi: 10.1038/nature07736
96	Feng B. J. ; Zhang J. ; Zhong Q. ; Li W. B. ; Li S. ; Li H. ; Cheng P. ; Meng S. ; Chen L. ; Wu K. H. Nat. Chem. 2016, 8, 563. doi: 10.1038/nchem.2491
97	Zhang X. X. ; Wu T. W. ; Wang H. B. ; Zhao R. B. ; Chen H. Y. ; Wang T. ; Wei P. P. ; Luo Y. L. ; Zhang Y. N. ; Sun X. P. ACS Catal. 2019, 9, 4609. doi: 10.1021/acscatal.8b05134
98	Minakshi M. ; Blackford M. G. Mater. Chem. Phys. 2010, 123, 700. doi: 10.1016/j.matchemphys.2010.05.041
99	Lv H. F. ; Peng T. ; Wu P. ; Pan M. ; Mu S. C. J. Mater. Chem. 2012, 22, 9155. doi: 10.1039/c2jm30538k
100	Mu S. C. ; Chen X. ; Sun R. H. ; Liu X. B. ; Wu H. ; He D. P. ; Cheng K. Carbon 2016, 103, 449. doi: 10.1016/j.carbon.2016.03.044
101	Song S. ; Xu W. ; Cao R. G. ; Luo L. L. ; Engelhard M. H. ; Bowden M. E. ; Liu B. ; Estevez L. ; Wang C. M. ; Zhang J. G. Nano Energy 2017, 33, 195. doi: 10.1016/j.nanoen.2017.01.042
102	Golberg D. ; Bando Y. ; Huang Y. ; Terao T. ; Mitome M. ; Tang C. C. ; Zhi C. Z. ACS Nano 2010, 4, 2979. doi: 10.1021/nn1006495
103	Zeng H. B. ; Zhi C. Y. ; Zhang Z. Z. ; Wei X. L. ; Wang X. B. ; Guo W. L. ; Bando Y. ; Golberg D. Nano Lett. 2010, 10, 5049. doi: 10.1021/nl103251m
104	Zhang Y. ; Du H. T. ; Ma Y. J. ; Ji L. ; Guo H. R. ; Tian Z. Q. ; Chen H. Y. ; Huang H. ; Cui G. W. ; Asiri A M. ; et al Nano Res. 2019, 12, 919. doi: 10.1007/s12274-019-2323-x
105	Lee J. ; Kang J. J. Catal. 2019, 375, 68. doi: 10.1016/j.jcat.2019.05.018
106	Mao X. ; Zhou S. ; Yan C. ; Zhu Z. H. ; Du A. J. Phys. Chem. Chem. Phys. 2019, 21, 1110. doi: 10.1039/c8cp07064d
107	Yang B. C. ; Wan B. S. ; Zhou Q. H. ; Wang Y. ; Hu W. T. ; Lv W. M. ; Chen Q. ; Zeng Z. M. ; Wen F. S. ; Xiang J Y. ; et al Adv. Mater. 2016, 28, 9408. doi: 10.1002/adma.201603723
108	Kang J. ; Wells S. A. ; Wood J. D. ; Lee J. H. ; Liu X. L. ; Ryder C.R. ; Zhu J. ; Guest J. R. ; Husko C. A. ; Hersam M. C. Proc. Natl. Acad. Sci. USA 2016, 113, 11688. doi: 10.1073/pnas.1602215113
109	Yang D. ; Yang G. X. ; Yang P. P. ; Lv R. C. ; Gai S. L. ; Li C. X. ; He F. ; Lin J. Adv. Funct. Mater. 2017, 27, 1700371. doi: 10.1002/adfm.201700371
110	Kou L. Z. ; Frauenheim T. ; Chen C. F. J. Phys. Chem. Lett. 2014, 5, 2675. doi: 10.1021/jz501188k
111	Zhang L. L. ; Ding L. X. ; Chen G. F. ; Yang X. F. ; Wang H. H. Angew. Chem. Int. Ed. 2019, 58, 2612. doi: 10.1002/anie.201813174
112	Shi L. ; Li P. ; Zhou W. ; Wang T. ; Chang K. ; Zhang H. B. ; Kako T. ; Liu G. G. ; Ye J. H. Nano Energy 2016, 28, 158. doi: 10.1016/j.nanoen.2016.08.041
113	Chen Z. ; Zhao J. X. ; Yin L. C. ; Chen Z. F. J. Mater. Chem. A 2019, 7, 13284. doi: 10.1039/c9ta01410a
114	Zhou F. L. ; Azofra L. M. ; Ali M. ; Kar M. ; Simonov A. N. ; McDonnell-Worth C. ; Sun C. H. ; Zhang X. Y. ; MacFarlane D. R. Energy Environ. Sci. 2017, 10, 2516. doi: 10.1039/c7ee02716h
115	Zhu X. J. ; Wu T. W. ; Ji L. ; Li C. B. ; Wang T. ; Wen S. H. ; Gao S. Y. ; Shi X. F. ; Luo Y. L. ; Peng Q. L. ; Sun X. P. J. Mater. Chem. A 2019, 7, 16117. doi: 10.1039/c9ta05016g

[1]	Zehao Zhang, Zheng Wang, Haibo Li. Preparation of 2D V₂O₃@Pourous Carbon Nanosheets Derived from V₂CF_x MXene for Capacitive Desalination [J]. Acta Phys. -Chim. Sin., 2024, 40(8): 2308020-.
[2]	Xinyi Zhang, Kai Ren, Yanning Liu, Zhenyi Gu, Zhixiong Huang, Shuohang Zheng, Xiaotong Wang, Jinzhi Guo, Igor V. Zatovsky, Junming Cao, Xinglong Wu. Progress on Entropy Production Engineering for Electrochemical Catalysis [J]. Acta Phys. -Chim. Sin., 2024, 40(7): 2307057-.
[3]	Wencheng Fang, Dong Liu, Ying Zhang, Hao Feng, Qiang Li. Improved Photoelectrochemical Performance by Polyoxometalate-Modified CuBi₂O₄/Mg-CuBi₂O₄ Homojunction Photocathode [J]. Acta Phys. -Chim. Sin., 2024, 40(2): 2304006-.
[4]	Yao Chen, Cun Chen, Xuesong Cao, Zhenyu Wang, Nan Zhang, Tianxi Liu. Recent Advances in Defect and Interface Engineering for Electroreduction of CO₂ and N₂ [J]. Acta Phys. -Chim. Sin., 2023, 39(8): 2212053-0.
[5]	Ruifang Wei, Dongfeng Li, Heng Yin, Xiuli Wang, Can Li. Operando Electrochemical UV-Vis Absorption Spectroscopy with Microsecond Time Resolution [J]. Acta Phys. -Chim. Sin., 2023, 39(2): 2207035-0.
[6]	Qi Yuan, Hao Yang, Miao Xie, Tao Cheng. Theoretical Research on the Electroreduction of Carbon Dioxide [J]. Acta Phys. -Chim. Sin., 2021, 37(5): 2010040-.
[7]	Piao Jin, Zichao Guan, Yan Liang, Kai Tan, Xia Wang, Guangling Song, Ronggui Du. Photocathodic Protection on Stainless Steel by Heterostructured NiO/TiO₂ Nanotube Array Film with Charge Storage Capability [J]. Acta Phys. -Chim. Sin., 2021, 37(3): 1906033-.
[8]	Peng Zhou,Jinzhi Sheng,Chongwei Gao,Jun Dong,Qinyou An,Liqiang Mai. Synthesis of V₂O₅/Fe₂V₄O₁₃ Nanocomposite Materials using In situ Phase Separation and the Electrochemical Performance for Sodium Storage [J]. Acta Physico-Chimica Sinica, 2020, 36(5): 1906046-.
[9]	Chunhe YANG,Aiwei TANG,Feng TENG,Kejian JIANG. Electrochemistry of Perovskite CH₃NH₃PbI₃ Crystals [J]. Acta Phys. -Chim. Sin., 2018, 34(11): 1197-1201.
[10]	Yi-Fan RUAN,Nan ZHANG,Yuan-Cheng ZHU,Wei-Wei ZHAO,Jing-Juan XU,Hong-Yuan CHEN. New Developments in Photoelectrochemical Bioanalysis [J]. Acta Phys. -Chim. Sin., 2017, 33(3): 476-485.
[11]	Wei-Xin SONG,Hong-Shuai HOU,Xiao-Bo JI. Progress in the Investigation and Application of Na₃V₂(PO₄)₃ for Electrochemical Energy Storage [J]. Acta Phys. -Chim. Sin., 2017, 33(1): 103-129.
[12]	Lin LIU,Zhi-Sheng LI,Hui-Dong HU,Wei-Li SONG. Insight into Macroscopic Metal-Assisted Chemical Etching for Silicon Nanowires [J]. Acta Phys. -Chim. Sin., 2016, 32(4): 1019-1028.
[13]	Jing-Mei LÜ,Xuan CHENG. Electrochemical Behavior of Porous and Flat Silicon Electrode Interfaces [J]. Acta Phys. -Chim. Sin., 2016, 32(3): 711-716.
[14]	Juan XU,Jia-Qin LIU,Jing-Wei LI,Yan WANG,Jun Lü,Yu-Cheng WU. Controlled Synthesis and Supercapacitive Performance of Heterostructured MnO₂/H-TiO₂ Nanotube Arrays [J]. Acta Phys. -Chim. Sin., 2016, 32(10): 2545-2554.
[15]	Jia-Xu LIANG,Zhi-Chang XIAO,Lin-Jie ZHI. Graphenal Polymers: 3D Carbon-Rich Polymers as Energy Materials with Electronic and Ionic Transport Pathways [J]. Acta Phys. -Chim. Sin., 2016, 32(10): 2390-2398.

Recent Progress in Metal-Free Electrocatalysts toward Ambient N₂ Reduction Reaction

RichHTML

PDF

Like

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 15

References 115

Related Articles 15

Metrics

Recommended 0

Recent Progress in Metal-Free Electrocatalysts toward Ambient N2 Reduction Reaction

RichHTML

PDF

Like

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 15

References 115

Related Articles 15

Metrics

Recommended 0

Recent Progress in Metal-Free Electrocatalysts toward Ambient N₂ Reduction Reaction