Supporting Information. Engineering Two-Dimensional Mass-Transport Channels
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1 Supporting Information Engineering Two-Dimensional Mass-Transport Channels of MoS 2 Nanocatalyst towards Improved Hydrogen Evolution Performance Ge Wang a, Jingying Tao a, Yijie Zhang a, Shengping Wang a, Xiaojun Yan a, Congcong Liu a, Fei Hu a, Zhiying He a, Zhijun Zuo b, *, Xiaowei Yang a, * a Institute for Regenerative Medicine, Shanghai East Hospital, School of Materials Science and Engineering, Tongji University, Shanghai , China. b Key Laboratory of Coal Science and Technology of Ministry of Education and Shanxi Province, Taiyuan University of Technology, Taiyuan , Shanxi, China Corresponding Author * yangxw@tongji.edu.cn; zuozhijun@tyut.edu.cn. S-1
2 Figure S1. Characterization of the synthesized MoS 2 powders. (a) TEM image; (b) XRD pattern; (c, d) XPS scans for the Mo and S binding energies. S-2
3 Figure S2. The mechanism of the structural formation of channel-engineered MoS 2. Figure S3. SEM image of the cross-section of channel-engineered MoS 2. S-3
4 Figure S4. TEM image of carbon black. Figure S5. The HER performance of Pt/C, MS/C and MS. S-4
5 Figure S6. Cyclic voltammetry curves of MS (a) and MS/C (b) in the region of V vs SCE. Figure S7. Cyclic voltammetry curves of carbon black (a) and its plot of the extraction of C dl (b). S-5
6 Figure S8. Corresponding Randles equivalent circuit model of these MoS 2 electrode. Figure S9. The comparison of electrocatalytic properties between MS/Si, MS/C and MS. S-6
7 Figure S10. Durability test for the MS/C via cyclic voltammetry and chronopotentiometry curves (inset) at constant current densities of 100 ma cm -2. Figure S11. Comparison of overpotential and Tafel slope at the 2D substrate with other recently reported promising MoS 2 nanocatalysts. S-7
8 Figure S12. Comparison of overpotential and Tafel slope at 3D substrate with other recently reported promising MoS 2 nanocatalysts. Table S1. The R s, R i and R ct of MS and MS/C. R s (Ω) R i (Ω) R ct (Ω) MS MS/C S-8
9 Table S2. Comparison of the HER performance with other recently reported promising MoS 2 nanocatalysts at 2D electrode. Loading (mg cm -2 ) j (ma cm -2 ) (η = 227mV) Tafel slope (mv decade -1 ) Year MS/C This work MoS 2 nanoparticles/graphene ~45 ~ Amorphous MoS ~ Conducting MoS 2 nanosheets ~15 ~ Disorder engineered and oxygen-incorporated MoS Edge-terminated MoS Metallic phase MoS 2 nanosheets ~ Edge-oriented and Interlayer expanded MoS 2 /rgo ~ Nitrogen doped MoS 2 nanosheets ~ Size-controlled MoS 2 nanodots supported on ~ reduced graphene oxide 9 Amorphous MoS 2 /CNTs S-9
10 Table S3. Comparison of the HER performance with other recently reported promising MoS 2 nanocatalysts at 3D electrode. Loading (mg cm -2 ) j (ma cm -2 ) (η = 191mV) Tafel slope (mv decade -1 ) Year MS/C-CP This work Li-tuning vertical aligned MoS 2 /CFP MoS 2 /N-doped CNT forest Amorphous MoS x Cl y /vertical graphene growth at graphit disk 13 Basal planes activated and S- terminated MoS 2 /CC Stepped edge engineered MoS 2 /CFP MoS 2 grown on graphene/cfp MoS x /Ni foam MoS 2 nanoparticles/carbon nanofiber foam MoS 2 /CPs MoS 2 /vertical graphene on CC S-10
11 References: (1) Li, Y.; Wang, H.; Xie, L.; Liang, Y.; Hong, G.; Dai, H., MoS 2 Nanoparticles Grown on Graphene: An Advanced Catalyst for the Hydrogen Evolution Reaction. J. Am. Chem. Soc. 2011, 133, (2) Benck, J. D.; Chen, Z.; Kuritzky, L. Y.; Forman, A. J.; Jaramillo, T. F., Amorphous Molybdenum Sulfide Catalysts for Electrochemical Hydrogen Production: Insights into the Origin of their Catalytic Activity. ACS Catal. 2012, 2, (3) Voiry, D.; Salehi, M.; Silva, R.; Fujita, T.; Chen, M.; Asefa, T.; Shenoy, V. B.; Eda, G.; Chhowalla, M., Conducting MoS 2 Nanosheets as Catalysts for Hydrogen Evolution Reaction. Nano Lett. 2013, 13, (4) Xie, J.; Zhang, J.; Li, S.; Grote, F.; Zhang, X.; Zhang, H.; Wang, R.; Lei, Y.; Pan, B.; Xie, Y., Controllable Disorder Engineering in Oxygen-Incorporated MoS 2 Ultrathin Nanosheets for Efficient Hydrogen Evolution. J. Am. Chem. Soc. 2013, 135, (5) Gao, M. R.; Chan, M. K.; Sun, Y., Edge-Terminated Molybdenum Disulfide with a 9.4-Å Interlayer Spacing for Electrochemical Hydrogen Production. Nat. Commun. 2015, 6, (6) Geng, X.; Sun, W.; Wu, W.; Chen, B.; Al-Hilo, A.; Benamara, M.; Zhu, H.; Watanabe, F.; Cui, J.; Chen, T. P., Pure and Stable Metallic Phase Molybdenum Disulfide Nanosheets for Hydrogen Evolution Reaction. Nat. Commun. 2016, 7, (7) Sun, Y.; Alimohammadi, F.; Zhang, D.; Guo, G., Enabling Colloidal Synthesis of Edge- Oriented MoS 2 with Expanded Interlayer Spacing for Enhanced HER Catalysis. Nano Lett. 2017, 17, S-11
12 (8) Li, R.; Yang, L.; Xiong, T.; Wu, Y.; Cao, L.; Yuan, D.; Zhou, W., Nitrogen Doped MoS 2 Nanosheets Synthesized via a Low-Temperature Process as Electrocatalysts with Enhanced Activity for Hydrogen Evolution Reaction. J. Power Sources 2017, 356, (9) Sun, W.; Li, P.; Liu, X.; Shi, J.; Sun, H.; Tao, Z.; Li, F.; Chen, J., Size-Controlled MoS 2 Nanodots Supported on Reduced Graphene Oxide for Hydrogen Evolution Reaction and Sodium-Ion Batteries. Nano Res. 2017, 10, (10) Ye, Z.; Yang, J.; Li, B.; Shi, L.; Ji, H.; Song, L.; Xu, H., Amorphous Molybdenum Sulfide/Carbon Nanotubes Hybrid Nanospheres Prepared by Ultrasonic Spray Pyrolysis for Electrocatalytic Hydrogen Evolution. Small 2017, 13, (11) Wang, H.; Lu, Z.; Xu, S.; Kong, D.; Cha, J. J.; Zheng, G.; Hsu, P. C.; Yan, K.; Bradshaw, D.; Prinz, F. B.; Cui, Y., Electrochemical Tuning of Vertically Aligned MoS 2 Nanofilms and Its Application in Improving Hydrogen Evolution Reaction. Proc. Natl. Acad. Sci. U. S. A. 2013, 110, (12) Li, D. J.; Maiti, U. N.; Lim, J.; Choi, D. S.; Lee, W. J.; Oh, Y.; Lee, G. Y.; Kim, S. O., Molybdenum Sulfide/N-Doped CNT Forest Hybrid Catalysts for High-Performance Hydrogen Evolution Reaction. Nano Lett. 2014, 14, (13) Zhang, X.; Meng, F.; Mao, S.; Ding, Q.; Shearer, M. J.; Faber, M. S.; Chen, J.; Hamers, R. J.; Jin, S., Amorphous MoS x Cl y Electrocatalyst Supported by Vertical Graphene for Efficient Electrochemical and Photoelectrochemical Hydrogen Generation. Energy Environ. Sci. 2015, 8, S-12
13 (14) Huang, X.; Leng, M.; Xiao, W.; Li, M.; Ding, J.; Tan, T. L.; Lee, W. S. V.; Xue, J., Activating Basal Planes and S-Terminated Edges of MoS 2 toward More Efficient Hydrogen Evolution. Adv. Funct Mater. 2017, 27, (15) Hu, J.; Huang, B.; Zhang, C.; Wang, Z.; An, Y.; Zhou, D.; Lin, H.; Leung, M. K. H.; Yang, S., Engineering Stepped Edge Surface Structures of MoS 2 Sheet Stacks to Accelerate the Hydrogen Evolution Reaction. Energy Environ. Sci. 2017, 10, (16) Chang, Y. H.; Lin, C. T.; Chen, T. Y.; Hsu, C. L.; Lee, Y. H.; Zhang, W.; Wei, K. H.; Li, L. J., Highly Efficient Electrocatalytic Hydrogen Production by MoS x Grown on Graphene- Protected 3D Ni foams. Adv. Mater. 2013, 25, (17) Guo, X.; Cao, G. L.; Ding, F.; Li, X.; Zhen, S.; Xue, Y. F.; Yan, Y. M.; Liu, T.; Sun, K. N., A Bulky and Flexible Electrocatalyst for Efficient Hydrogen Evolution Based on the Growth of MoS 2 Nanoparticles on Carbon Nanofiber Foam. J. Mater. Chem. A 2015, 3, (18) Ye, T. N.; Lv, L. B.; Xu, M.; Zhang, B.; Wang, K. X.; Su, J.; Li, X. H.; Chen, J. S., Hierarchical Carbon Nanopapers Coupled with Ultrathin MoS 2 Nanosheets: Highly Efficient Large-Area Electrodes for Hydrogen Evolution. Nano Energy 2015, 15, (19) Zhang, Z.; Li, W.; Yuen, M. F.; Ng, T. W.; Tang, Y.; Lee, C. S.; Chen, X.; Zhang, W., Hierarchical Composite Structure of Few-Layers MoS 2 Nanosheets Supported by Vertical Graphene on Carbon Cloth for High-Performance Hydrogen Evolution Reaction. Nano Energy 2015, 18, S-13
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