Supplementary Figure 1 Morphology and composition of the original carbon nanotube (CNT) sample. (a, b) TEM images of CNT; (c) EDS of CNT.
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1 1 Supplementary Figure 1 Morphology and composition of the original carbon nanotube (CNT sample. (a, b TEM images of CNT; (c EDS of CNT. Cobalt is not detected in the original CNT sample (Note: The accidentally detected signal of Si is from the EDS detector. Scale bar, 1 nm (a; 2 nm (b.
2 2 a b Supplementary Figure 2 (a, b TEM images of the CoPc/CNT(26% hybrid. Wrinkles are observed at the edge of nanotubes, which might correspond to the CoPc molecule aggregates. Scale bar, 1 nm (a; 2 nm (b.
3 3 a b Supplementary Figure 3 (a, b TEM images of the CoPc/CNT(2.5% hybrid. The CNT sidewalls appear smooth, indicating that CoPc is possibly dispersed on molecular level. Scale bar, 1 nm (a; 2 nm (b.
4 4 CoPc/CNT(26% CoPc/CNT(6.% CoPc/CNT(2.5% CoPc/CNT(.5% Intensity (a.u Wavenumber (cm -1 Supplementary Figure 4 Raman spectra of the CoPc/CNT(26%, CoPc/CNT(6%, CoPc/CNT(2.5%, and CoPc/CNT(.5% hybrids.
5 5 a b CoPc (Ar CoPc (CO 2 CNT (Ar CNT (CO 2 CoPc-CNT 6% (Ar CoPc-CNT 6% (CO CFP (Ar CFP (CO 2 CoPc (Ar CoPc (CO E (V vs. RHE E (V vs. RHE Supplementary Figure 5 Cyclic voltammograms in.2 M aqueous phosphate buffer (ph 7.2. The data were recorded at a scan rate of 5 mv s -1 and the solutions were saturated with Ar (dashed line or CO 2 (solid line. (a CoPc/CNT(6% hybrid catalyst, CoPc (.2 mg cm -2, and CNT. (b CoPc (.4 mg cm -2 and bare carbon fiber paper (CFP substrate. The data are all ir corrected.
6 E (V vs. RHE CoPc/CNT (26% (Ar CoPc/CNT (26% (CO 2 CoPc/CNT (6% (Ar CoPc/CNT (6% (CO 2 CoPc/CNT (2.5% (Ar CoPc/CNT (2.5% (CO 2 CoPc/CNT (.5% (Ar CoPc/CNT (.5% (CO 2 CoPc-CN/CNT (3.5% (Ar CoPc-CN/CNT (3.5% (CO 2 Supplementary Figure 6 Cyclic voltammograms of the hybrids with various content. The data were recorded in.2 M aqueous phosphate buffer (ph 7.2 saturated with Ar (dashed line or CO 2 (solid line at a scan rate of 5 mv s -1 for the CoPc/CNT(26%, CoPc/CNT(6%, CoPc/CNT(2.5%, CoPc/CNT(.5% and CoPc-CN/CNT(3.5% hybrids. The reduction current increases with the CoPc percentage, but starts to saturate when the CoPc percentage goes over 2.5 wt%. The data are ir corrected.
7 7 a b Absorbance (a.u. Pc CoPc Intensity (a.u. Pc CoPc CoPc/CNTs after catalysis CoPc/CNTs after catalysis Wavelength (nm Wavelength (nm Supplementary Figure 7 Characterizations of the hybrid after electrocatalysis. (a UV- Vis absorption and (b fluorescence spectra for pristine Pc, pristine CoPc, and CoPc after electrocatalyzing CO 2 reduction at -.57 V vs. RHE after 1 h. All measurements were performed on samples dispersed in DMF. For the hybrid sample after electrolysis, the molecules were re-dissolved in DMF from the electrode by sonication.
8 8 a. b V V V V c Time (s Time (s -.46V -.53V V V Time (s Supplementary Figure 8 Chronoamperograms for electrochemical CO 2 reduction in CO 2 saturated.1 M KHCO 3 for 1 h at different potentials. (a CNT sample. (b CoPc (.2 mg cm -2. (c CoPc (.4 mg cm -2.
9 9 Supplementary Figure 9 Morphology and composition of the CoPc-CN/CNT hybrid sample. (a, b TEM images of the CoPc-CN/CNT hybrid; (c EDS of CoPc-CN/CNT hybrid. Co signal is detected, suggesting the existence of CoPc-CN molecules. (Note: The accidentally detected signal of Si is from the EDS detector. Scale bar, 1 nm (a; 2 nm (b.
10 1 a b 1 II a I a II'a I' a CoPc/CNT CoPc-CN/CNT -1-2 II c I' c I c CoPc/CNT CoPc-CN/CNT E (V vs. RHE E (V vs. RHE Supplementary Figure 1 Cyclic voltammograms in.1 M aqueous KHCO 3 solution saturated with CO 2 at different scan rate. (a 5 mv s -1 and (b 4 mv s -1. The Co(II/Co(I redox transition (IIc/IIa is more obvious and positively shifted in CoPc-CN/CNT compared to CoPc/CNT.
11 11 a b V CoPc-CN/CNT V -.48 V c E (V vs. RHE Time (h 8 FE (% 6 4 H 2 CO E (V vs. RHE Supplementary Figure 11 Electrocatalytic performance of CoPc-CN/CNT in.5 M aqueous KHCO 3 solution saturated with CO 2. (a Cyclic voltammogram, (b Chronoamperograms and (c Faradaic efficiences of H 2 and CO. The average values and error bars in (c are based on six measurements during three reaction runs (two product analysis measurements were performed in each run. The error bars represent S.D. of six measurements. The data are all ir corrected.
12 12 a CoPc aggregate b CoPc aggregate Supplementary Figure 12 SEM images of CoPc directly loaded on CFP. Samples prepared by drop-drying CoPc dispersed in (a ethanol and (b DMF. Scale bar, 4 μm (a, b.
13 E (V vs. RHE Supplementary Figure 13 Cyclic voltammogram for CoPc directly loaded on CFP from DMF. The electrode was prepared by drop-drying from the CoPc/DMF dispersion (loading:.2 mg cm -2. The data were recorded in.1 M aqueous KHCO 3 solution saturated with CO 2 at 5 mv s -1 with ir correction on the potential. Outflow of gas products
14 Supplementary Figure 14 Digital photos of the electrocatalytic measurement system. 14
15 15 Supplementary Table 1 Contents of phthalocyanine molecules in the hybrid catalysts determined by ICP-MS. Initial CoPc/carbon weight ratio before mixing Mass percentage of CoPc in the hybrid (% Denoted in the paper CoPc/CNT = 1:2 26 CoPc/CNT(26% CoPc/CNT = 1:8 6. CoPc/CNT(6% CoPc/CNT = 1:2 2.5 CoPc/CNT(2.5% CoPc/CNT = 1:1.48 CoPc/CNT(.5% CoPc/CB = 1:8 3.3 CoPc/CB(3.3% CoPc/RGO = 1:3 2.2 CoPc/RGO(2.2%
16 16 Supplementary Table 2 Calculated turnover frequency (TOF of CO 2 reduction to CO for the electrocatalysts in CO 2 -saturated.1 M aqueous KHCO 3. Sample name TOF(s -1 at V TOF(s -1 at V CoPc (±.1.22 (±.2 CoPc (±.1.22 (±.1 CoPc/CNT (26%.22 (±..15 (±. CoPc/CNT (6%.97 (±..66 (±. CoPc/CNT (2.5% 2.7 (±. 1.7 (±. CoPc/CB (3%.56 (±.1.32 (±.1 CoPc/RGO (2%.93 (±.2.42 (±.2 CoPc-CN/CNT (3.5% 4.1 (±.1 3. (±.
17 17 Supplementary Table 3 Summary of catalyst electrode potentials with and without ir correction. Sample CoPc/CNT (2.5% TOF CoPc-CN/CNT (3.5% CV, TOF CoPc-CN/CNT (3.5% CV, TOF CoPc-.2 mg cm -2 CV, TOF CoPc-.4 mg cm -2 CV, TOF CoPc/CNT (26% (CV, TOF CoPc/CNT (6% (CV, TOF CoPc/CNT (2.5% (CV CoPc/CB (3% CV, TOF CoPc/RGO (2% CV, TOF CNT CV Pc/CNT CV Electrolyte (ph.5m KHCO 3 (7.2 Resistance (Ω Corrected Potentials (V Original Potentials (V
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