Pt-like Hydrogen Evolution Electrocatalysis on PANI/CoP Hybrid Nanowires. by Weakening the Shackles of Hydrogen Ions on the Surfaces of Catalysts
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1 Pt-like Hydrogen Evolution Electrocatalysis on PANI/CoP Hybrid Nanowires by Weakening the Shackles of Hydrogen Ions on the Surfaces of Catalysts Jin-Xian Feng, Si-Yao Tong, Ye-Xiang Tong, and Gao-Ren Li * MOE Laboratory of Bioinorganic and Synthetic Chemistry, The Key Lab of Low-carbon Chemistry & Energy Conservation of Guangdong Province, School of Chemistry, Sun Yat-sen University, Guangzhou 5275, China Zhixin High School, Guangzhou 5080, China ligaoren@mail.sysu.edu.cn Scheme S1. The fabrication process of PANI/CoP HNWs-CFs electrocatalysts. 1
2 Figure S1. SEM image of CFs. Figure S2. (a) SEM image of Co(OH)2 NWs-CFs; (b) TEM image of a Co(OH)2 NW. 2
3 Figure S3. SEM image CoP NWs-CFs (Inset: TEM image of a CoP NW). 3
4 a Absorbance/a.u. C-C PANI/CoP HNWs-CFs 1492 para-substituted N-H C-H 3024 C=C Benzene rings vibrations Parasubstituted C-N N=Q=N rings vibrations b Intensity/a.u. Co 2p 3/ Sat. Co 2p Co 2p 1/ Sat Co 2+ in CoPO x Co in CoP Wavenumber/cm -1 Binding energy/ev c Intensity/a.u. PANI/CoP HNWs-CFs P in CoP P 2p 3/ P 2p 1/ P 2p P in surface CoPO x d Intensity/a.u. -NH N= N N 1s PANI/CoP HNWs-CFs Binding energy/ev Binding energy/ev Figure S4. (a) FT-IR spectra of PANI/CoP HNWs-CFs; (b-d) XPS spectra of (b) Co 2p, (c) P 2p and (d) N 1s of PANI/CoP HNWs-CFs. 4
5 Figure S5. SEM image of PANI NDs-CFs. (a) Current density/ma cm -2 0 CoP NWs-CFs PANI/CoP=0.25 PANI/CoP=0. - PANI/CoP=0.15 PANI/CoP= PANI/CoP= Potential/V vs. RHE (b) 24 j a -j c /ma cm PANI/CoP=0.05 PANI/CoP=0. PANI/CoP=0.15 PANI/CoP=0. PANI/CoP= Scan rate/mv s -1 Figure S6. (a) HER polarization curves of PANI/CoP HNWs-CFs with different PANI/CoP mass ratios; (b) Charging current density differences j a -j c plotted against the scan rates of PANI/CoP HNWs-CFs with different mass ratios of PANI/CoP.
6 Current density/ma cm mg cm mg cm mg cm mg cm mg cm mg cm Potential/V vs. RHE Figure S7. Relationship between the catalytic activity and loading mass of PANI/CoP HNWs-CFs. Current density/a g mg cm -2 PANI NDs mg cm mg cm -2 CoP NWs PANI/CoP HNWs Potential/V vs. RHE Figure S8. HER polarization curves of PANI NDs-CFs, CoP NWs-CFs and PANI/CoP HNWs-CFs based on loading masses. 6
7 0.16 PANI/CoP HNWs-CFs CoP NWs-CFs Overpotential/V mv/dec 46.3 mv/dec Log(j/mA.cm -2 ) Figure S9. Tafel plots of PANI/CoP HNWs-CFs and CoP NWs-CFs. j a -j c /ma cm PANI/CoP HNWs-CFs PANI NDs-CFs CoP NWs-CFs mf cm mf cm mf cm Scan rate/mv s -1 Figure S. Charging current density differences j a -j c plotted against the scan rates of PANI NDs-CFs, CoP NWs-CFs and PANI/CoP HNWs-CFs electrocatalysts. 7
8 Figure S11. SEM image of PANI/CoP HNWs-CFs after HER at V for 30 h (Inset: TEM image of CoP NW). After HER electrocatalysis Before HER electrocatalysis Potonated N=Q=N Intensity/a.u. -OH -NH + 2 Benzene rings vibrations H 2 O C-C C-N + C=C Wavenumber/cm -1 Figure S12. FT-IR spectra of PANI/CoP HNWs-CFs before and after HER at V for 30 h. 8
9 Intensity/a.u. Amorphous PANI * (011) (111) (2) * * * (112) (211) Before 30 h HER After 30 h HER (301) * * * * PANI * CoP θ/degree Figure S13. XRD patterns of PANI/CoP HNWs-CFs after HER at V for 30 h. 9
10 a b Figure S14. Hydride proton H 13 O 6 + (a) and (b) Protonated PANI model.
11 a b c d Figure S15. Models of (a) CoP-H 13 O 6 + ; (b) CoP-H + +6H 2 O; (c) CoP/PANI-H + +6H 2 O; and (d) CoP-H + / PANI+6H 2 O. 11
12 a b c Figure S16. Simplified CoP cluster: (a) front view (b) top view, and (c) side view. Figure S17. Simplified PANI cluster. 12
13 a b Figure S18. Simplified PANI/CoP cluster (a) front view and (b) side view. Current density/ma cm -2 0 CoP NWs-CFs (1.0 M PBS ph=7) PANI/CoP HNWs-CFs (1.0 M PBS ph=7) CoP NWs-CFs (0.5 M H 2 SO 4 ) PANI/CoP HNWs-CFs (0.5 M H 2 SO 4 ) Potential/V vs. RHE Figure S19. Polarization curves of CoP NWs-CFs and PANI/CoP HNWs-CFs electrocatalysts in ph=7 media (1.0 M PBS) and 0.5 M H 2 SO 4. 13
14 Table S1. Comparisons of the electrocatalytic activity of PANI/CoP HNWs-CFs catalysts in acidic media vis-à-vis some representative solid-state HER catalysts recently reported. (U: Onset potential; η j : Overpotential at the applied current density; j: Current density). Electrocatalyst PANI/CoP HNWs-CFs Loading/mg cm -2 U/mV η j /mv j/ma.cm -2 Reference CoP/CC Our work Ref 1 CoP NPs/Ti Ref 2 CoP NSs/Ti Ref 3 Urchin-like CoP NCs Ref 4 0 MoP S Ref CoP@NC Ref 6 FeP NA/Ti Ref 7 Co 2 P@NPG Ref 8 Cu 3 P NW/CF Ref MoP-CA Ref
15 Ni 5 P 4 films Ref 11 Nanostructured Ni 2 P Ref 12 CoS 2 /RGO-CNT film Ref 13 CoNi@NC Ref 14 WS 2 /WO 2.9 /C Ref CoSe 2 nanoparticles Ref Defect-rich MoS 2 ultrathin nanosheets Ref 17 Fe 0.9 Co 0.1 S 2 /CNT Ref 18 MoS 2 /CoSe Ref 19 Core-shell NiAu/Au Ref α-ins ultrathin nanosheets Ref 21 MoP@RGO Ref 22 WO Ref 23 CoMoS Ref 24 Pt-TaS Ref 25
16 190 Co 9 S 2 /CNFs Ref Ni-doped graphene Ref Ni-C-N nanosheets Ref Co-C-N complex Ref WO 2 -carbon 138 mesoporous Ref 30 nanowires Pt@CIAC Ref 31 16
17 Table S2. Comparisons of the long-term stability of the PANI/CoP HNWs-CFs catalysts under the acidic conditions vis-à-vis some representative solid-state HER catalysts recently reported. η o : Applied overpotential; j i : initial current density; j f : final constant current density. Electrocatalyst Loading/ mg cm -2 Reaction time/h Electrochemical performance j i =19.2 ma/cm 2 η 0 =50 mv j f =18.8 ma/cm 2 Reference PANI/CoP HNWs-CFs η 0 =75 mv η 0 =0 mv j i =32.0 ma/cm 2 j f =31.0 ma/cm 2 j i =53.1 ma/cm 2 j f =52.9 ma/cm 2 Our work η 0 =1 mv j i =87.9 ma/cm 2 j f =86.4 ma/cm 2 CoP NSs/Ti η 0 =150 mv j i =1 ma/cm 2 j f =1 ma/cm 2 Ref 3 Urchin-like CoP NCs η 0 =150 mv j i =1 ma/cm 2 j f =1 ma/cm 2 Ref 4 Cu 3 P NW/CF η 0 =0 mv j i =28mA/cm 2 j f =28 ma/cm 2 Ref 9 Co 2 P@NPG η 0 =0 mv η 0 =150 mv j i =6.3 ma/cm 2 j f =6 ma/cm 2 j i =25 ma/cm 2 j f =23 ma/cm 2 Ref 8 MoP-CA η 0 =150 mv WS 2 /WO 2.9 /C η 0 =1 mv j i =27 ma/cm 2 j f =25 ma/cm 2 Ref j i =11 ma/cm 2 j f = ma/cm 2 Ref 15 CoSe 2 nanoparticles η 0 =155 mv η 0 =173 mv j i = ma/cm 2 j f = ma/cm 2 j i =50 ma/cm 2 Ref 16 17
18 η 0 =185 mv j f =45 ma/cm 2 j i =0 ma/cm 2 j f =95 ma/cm 2 Defect-rich MoS 2 ultrathin nanosheets η 0 =0 mv j i =13 ma/cm 2 j f =12.5 ma/cm 2 Ref 17 Fe 0.9 Co 0.1 S 2 /CNT η 0 =1 mv MoS 2 /CoSe η 0 =700 mv WO η 0 =0 mv CoMoS η 0 =170 mv j i =21 ma/cm 2 j f = ma/cm 2 Ref 18 j i =150 ma/cm 2 j f =250 ma/cm 2 Ref 19 j i =.2 ma/cm 2 j f =19 ma/cm 2 Ref 23 j i =12 ma/cm 2 j f =4 ma/cm 2 Ref 24 Co 9 S 2 /CNFs Ni-doped graphene η 0 =190 mv η 0 =150 mv j i =18 ma/cm 2 j f =23 ma/cm 2 Ref 26 j i =9.2 ma/cm 2 j f =9.2 ma/cm 2 Ref 27 Co-C-N complex η 0 =1 mv j i =21 ma/cm 2 j f = ma/cm 2 Ref 29 References (1) Tian, J.; Liu, Q.; Asiri, A.; Sun, X. J. Am. Chem. Soc. 14, 136, (2) Popczun, E.; Read, C.; Roske, C.; Lewis, N.; Schaak, R. Angew. Chem. Int. Ed. 14, 53, (3) Pu, Z.; Liu, Q.; Jiang, P.; Asiri, A.; Obaid, A.; Sun, X. Chem. Mater. 14, 26, (4) Yang, H.; Zhang, Y.; Hu, F.; Wang, Q. Nano Lett. 15, 15, (5) Kibsgaard, J.; Jaramillo, T. Angew. Chem. Int. Ed. 14, 53, (6) Yang, F.; Chen, Y.; Cheng, G.; Chen, S.; Luo, W. ACS Catal. 17, 7, (7) Jiang, P.; Liu, Q.; Liang, Y.; Tian, J.; Asiri, A.; Sun, X. Angew. Chem. Int. Ed. 14, 53, (8) Zhuang, M.; Ou, X.; Dou, Y.; Zhang, L.; Zhang, Q.; Wu, R.; Ding, Y.; Shao, M.; Luo, Z. Nano Lett. 16, 16, (9) Tian, J.; Liu, Q.; Cheng, N.; Asiri, A.; Sun, X. Angew. Chem. Int. Ed. 14, 53,
19 () Xing, Z.; Liu, Q.; Asiri, A.; Sun, X. Adv. Mater. 14, 26, (11) Ledendecker, M.; Calderón, S.; Papp, C.; Steinrîck, H.; Antonietti, M.; Shalom, M. Angew. Chem. Int. Ed. 15, 54, (12) Popczun, E.; McKone, J.; Read, C.; Biacchi, A.; Wiltrout, A.; Lewis, N.; Schaak, R. J. Am. Chem. Soc. 13, 135, (13) Peng, S.; Li, L.; Han, X.; Sun, W.; Srinivasan, M.; Mhaisalkar, S.; Cheng, F.; Yan, Q.; Chen, J.; Ramakrishna, S. Angew. Chem. Int. Ed. 14, 53, (14) Deng, J.; Ren, P.; Deng, D. Bao, X. Angew. Chem. Int. Ed. 15, 54,. (15) Wang, X.; Gan, X.; Hu, T.; Fujisawa, K.; Lei, Y.; Lin, Z.; Xu, B.; Huang, Z.; Kang, F.; Terrones, M.; Lv, R. Adv. Mater. 17, 29, (16) Kong, D.; Wang, H.; Lu, Z. Cui, Y. J. Am. Chem. Soc. 14, 136, (17) Xie, J.; Zhang, H.; Li, S.; Wang, R.; Sun, X.; Zhou, M.; Zhou, J.; Lou, X.; Xie, Y. Adv. Mater. 13, 25, (18) Wang, D.; Gong, M.; Chou, H.; Pan, C.; Chen, H.; Wu, Y.; Lin, M.; Guan, M.; Yang, J.; Chen, C.; Wang, Y.; Hwang, B.; Chen, C.; Dai, H. J. Am. Chem. Soc. 15, 137, (19) Gao, M.; Liang, J.; Zheng, Y.; Xu, Y.; Jiang, J.; Gao, Q.; Li, J.; Yu, S. Nat. Commun. 15, 6, () Lv, H.; Xi, Z.; Chen, Z.; Guo, S.; Yu, Y.; Zhu, W.; Li, Q.; Zhang, X.; Pan, M.; Lu, G.; Mu, S.; Sun, S. J. Am. Chem. Soc. 15, 137, (21) Long, X.; Li, G.; Wang, Z.; Zhu, H.; Zhang, T.; Xiao, S.; Guo, W.; Yang, S. J. Am. Chem. Soc. 15, 137, (22) Zhang, G.; Wang, G.; Liu, Y.; Liu, H.; Qu, J.; Li, J. J. Am. Chem. Soc., 16, 138, (23) Li, Y.; Liu, P.; Pan, L.; Wang, H.; Yang, Z.; Zheng, L.; Hu, P.; Zhao, H.; Gu, L.; Yang, H. Nat. Commun. 15, 6, (24) Yu, L.; Xia, B.; Wang, X.; Lou, X. Adv. Mater. 16, 28, 92. (25) Zeng, Z.; Tan, C.; Huang, X.; Bao, S.; Zhang, H. Energy Environ. Sci. 14, 7, 797. (26) Zhu, H.; Zhang, J.; Yanzhang, R.; Du, M.; Wang, Q.; Gao, G.; Wu, J.; Wu, G.; Zhang, M.; Liu, B.; Yao, J.; Zhang, X. Adv. Mater. 15, 27, (27) Qiu, H.; Ito, Y.; Cong, W.; Tan, Y.; Liu, P.; Hirata, A.; Fujita, T.; Tang, Z.; Chen, M. Angew. Chem. Int. Ed. 15, 54, (28) Yin, J.; Fan, Q.; Li, Y.; Cheng, F.; Zhou, P.; Xi, P.; Sun, S. J. Am. Chem. Soc., 16, 138, (29) Wang, Z.; Hao, X.; Jiang, Z.; Sun, X.; Xu, D.; Wang, J.; Zhong, H.; Meng, F.; Zhang, X. J. Am. Chem. Soc., 15, 137, (30) Wu, R.; Zhang, J.; Shi, Y.; Liu, D.; Zhang, B. J. Am. Chem. Soc. 15, 137, (31) Wang, S.; Gao, X.; Hang, X.; Zhu, X.; Han, H.; Liao, W.; Chen, W. J. Am. Chem. Soc. 16, 138,
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