Page 7 of 16
Journal of the American Chemical Society
(7) Shan, J. J.; Li, M. W.; Allard, L. F.; Lee, S.; Flytzani-
The details of the XAFS analysis and theoretical
calculations are shown in the Supporting Information.
Stephanopoulos, M., Mild oxidation of methane to methanol or
acetic acid on supported isolated rhodium catalysts. Nature 2017,
551, 605-608.
1
2
3
4
5
6
7
8
ASSOCIATED CONTENT
*Supporting Information
The Supporting Information is available free of charge on
the ACS Publications website.
Detailed experimental procedures, characterization
methods, extended figures, and tables.
(8) Liu, P. X.; Zhao, Y.; Qin, R. X.; Mo, S. G.; Chen, G. X.; Gu, L.;
Chevrier, D. M.; Zhang, P.; Guo, Q.; Zang, D. D.; Wu, B. H.; Fu, G.;
Zheng, N. F., Photochemical route for synthesizing atomically
dispersed palladium catalysts. Science 2016, 352, 797-801.
(9) Liu, G. L.; Robertson, A. W.; Li, M. M.; Kuo, W. C. H.; Darby, M. T.;
Muhieddine, M. H.; Lin, Y. C.; Suenaga, K.; Stamatakis, M.; Warner, J.
H.; Tsang, S. C. E., MoS2 monolayer catalyst doped with isolated Co
atoms for the hydrodeoxygenation reaction. Nat. Chem. 2017, 9,
810-816.
(10) Yang, S.; Kim, J.; Tak, Y. J.; Soon, A.; Lee, H., Single-atom catalyst
of platinum supported on titanium nitride for selective
electrochemical reactions. Angew. Chem. Int. Ed. 2016, 55, 2058-
2062.
9
AUTHOR INFORMATION
Corresponding Author
*cchen@mail.tsinghua.edu.cn
Author Contributions
10
11
12
13
14
15
16
17
18
19
20
21
22
23
24
25
26
27
28
29
30
31
32
33
34
35
36
37
38
39
40
41
42
43
44
45
46
47
48
49
50
51
52
53
54
55
56
57
58
59
60
(11) Xia, Y.; Mathis, T. S.; Zhao, M. Q.; Anasori, B.; Dang, A.; Zhou, Z.
H.; Cho, H.; Gogotsi, Y.; Yang, S., Thickness-independent
capacitance of vertically aligned liquid-crystalline MXenes. Nature
2018, 557, 409-412.
∆ D. Z., Z. C. and W. J. Y. contributed equally.
Notes
(12) Ghidiu, M.; Lukatskaya, M. R.; Zhao, M. Q.; Gogotsi, Y.; Barsoum,
M. W., Conductive two-dimensional titanium carbide 'clay' with
high volumetric capacitance. Nature 2014, 516, 78-81.
(13) Lukatskaya, M. R.; Mashtalir, O.; Ren, C. E.; Dall’Agnese, Y.;
Rozier, P.; Taberna, P. L.; Naguib, M.; Simon, P.; Barsoum, M. W.;
Gogotsi, Y., Cation intercalation and high volumetric capacitance of
two-dimensional titanium carbide. Science 2013, 341, 1502-1505.
(14) Shahzad, F.; Alhabeb, M.; Hatter, C. B.; Anasori, B.; Hong, S. M.;
Koo, C. M.; Gogotsi, Y., Electromagnetic interference shielding with
2D transition metal carbides (MXenes). Science 2016, 353, 1137-
1140.
The authors declare no competing financial interest.
ACKNOWLEDGMENT
This work was supported by Beijing Natural Science
Foundation (JQ18007), National Key R&D Program of China
(2017YFA0700101, 2016YFA0202801), National Natural
Science Foundation of China (21872076, 21573119,
21590792, 51651201, 21866032, and 21805184), China
(15) Di, J.; Yan, C.; Handoko, A. D.; Seh, Z. W.; Li, H.; Liu, Z., Ultrathin
two-dimensional materials for photo- and electrocatalytic
hydrogen evolution. Mater. Today 2018, 21, 749-770.
(16) Handoko, A. D.; Fredrickson, K. D.; Anasori, B.; Convey, K. W.;
Johnson, L. R.; Gogotsi, Y.; Vojvodic, A.; Seh, Z. W., Tuning the basal
plane functionalization of two-dimensional metal carbides
(MXenes) to control hydrogen evolution activity. ACS Appl. Mater.
Interfaces 2017, 1, 173-180.
(17) Li, P. K.; Zhu, J. G.; Handoko, A. D.; Zhang, R. F.; Wang, H. T.;
Legut, D.; Wen, X. D.; Fu, Z. H.; Seh, Z. W.; Zhang, Q. F., High-
throughput theoretical optimization of the hydrogen evolution
reaction on MXenes by transition metal modification. J. Mater.
Chem. A 2018, 6, 4271-4278.
(18) Handoko, A. D.; Khoo, K. H.; Tan, T. L.; Jin, H. M.; Seh, Z. W.,
Establishing new scaling relations on two-dimensional MXenes for
CO2 electroreduction. J. Mater. Chem. A 2018, 6, 21885-21890.
(19) Zhang, J. Q.; Zhao, Y. F.; Guo, X.; Chen, C.; Dong, C. L.; Liu, R. S.;
Han, C. P.; Li, Y. D.; Gogotsi, Y.; Wang, G. X., Single platinum atoms
immobilized on an MXene as an efficient catalyst for the hydrogen
evolution reaction. Nat. Catal. 2018, 1, 985-992.
(20) Li, Z.; Cui, Y. R.; Wu, Z. W.; Milligan, C.; Zhou, L.; Mitchell, G.; Xu,
B.; Shi, E.; Miller, J. T.; Ribeiro, F. H.; Wu, Y., Reactive metal–support
interactions at moderate temperature in two-dimensional
niobium-carbide-supported platinum catalysts. Nat. Catal. 2018, 1,
349-355.
Postdoctoral
2018M631444, and 2018M631486) and the National
Postdoctoral Program for Innovative Talents
(BX201700131). We thank the 1W1B station for XAFS
measurements in the Beijing Synchrotron Radiation Facility
(BSRF). We thank Tsinghua National Laboratory for
Information Science and Technology for providing grid
resources that have contributed to calculation results. Also,
we thank Dr. C. Zhang for the help in preparing this
manuscript.
Science
Foundation
(2018M631445,
REFERENCES
(1) Wang, A. Q.; Li, J.; Zhang, T., Heterogeneous single-atom
catalysis. Nat. Rev. Chem. 2018, 2, 65-81.
(2) Liu, X. F.; Li, X. Y.; Qiao, C.; Fu, H. C.; He, L. N., Betaine catalysis
for hierarchical reduction of CO2 with amines and hydrosilane to
form formamides, aminals, and methylamines. Angew. Chem. Int.
Ed. 2017, 56, 7425-7429.
(3) Zhang, L.; Han, Z. B.; Zhao, X.; Wang, Z.; Ding, K. l., Highly
efficient ruthenium-catalyzed N-formylation of amines with H2 and
CO2. Angew. Chem. Int. Ed. 2015, 54, 6186-6189.
(4) Handoko, A. D.; Wei, F.; Jenndy; Yeo, B. S.; Seh, Z. W.,
Understanding heterogeneous electrocatalytic carbon dioxide
reduction through operando techniques. Nat. Catal. 2018, 1, 922-
934.
(5) Wei, S. J.; Li, A.; Liu, J. C.; Li, Z.; Chen, W. X.; Gong, Y.; Zhang, Q.
H.; Cheong, W. C.; Wang, Y.; Zheng, L. R.; Xiao, H.; Chen, C.; Wang, D.
S.; Peng, Q.; Gu, L.; Han, X. D.; Li, J.; Li, Y. D., Direct observation of
noble metal nanoparticles transforming to thermally stable single
atoms. Nat. Nanotechnol. 2018, 13, 856-861.
(6) Chen, Z. P.; Vorobyeva, E.; Mitchell, S.; Fako, E.; Ortuno, M. A.;
Lopez, N.; Collins, S. M.; Midgley, P. A.; Richard, S.; Vile, G.; Perez-
Ramirez, J., A heterogeneous single-atom palladium catalyst
surpassing homogeneous systems for Suzuki coupling. Nat.
Nanotechnol. 2018, 13, 702-707
(21) Xie, X. H.; Chen, S. G.; Ding, W.; Nie, Y.; Wei, Z. D., An
extraordinarily stable catalyst: Pt NPs supported on two-
dimensional Ti3C2X2 (X = OH, F) nanosheets for oxygen reduction
reaction. Chem. Commun. 2013, 49, 10112-10114.
(22) Zhang, Z. W.; Li, H. N.; Zou, G. D.; Fernandez, C.; Liu, B. D.;
Zhang, Q. R.; Hu, J.; Peng, Q. M., Self-reduction synthesis of new
MXene/Ag composites with unexpected electrocatalytic activity.
ACS Sustain. Chem. Eng. 2016, 4, 6763-6771.
(23) Anasori, B.; Lukatskaya, M. R.; Gogotsi, Y., 2D metal carbides
and nitrides (MXenes) for energy storage. Nat. Rev. mater. 2017, 2,
16098.
ACS Paragon Plus Environment