RECOMMENDED README FILE FOR DIGITAL.CSIC DATASETS GENERAL INFORMATION 1. Title of Dataset: Supplementary material of the article Molecular Engineering to Introduce Carbonyl Between Nickel Salophen Active Sites to Enhance Electrochemical CO2 Reduction to Methanol 2. Authors: Liang, Zhifu; Wang, Jianghao; Tang, Peng-Yi; Tang, Weiqiang; Liu, Lijia; Shakouri, Mohsen; Wang, Xiang; Llorca, Jordi; Zhao, Shuangliang; Heggen, Marc; Dunin-Borkowski, Rafal E.; Cabot, Andreu; Wu, Hao Bin; Arbiol, Jordi 3. Date of data collection: N/A 4. Date of data publication on repository: 2022-10-05 5. Geographic location of data collection : N/A 6. Information about funding sources that supported the collection of the data (including research project reference/acronym): ICN2 is supported by the Severo Ochoa program from Spanish MINECO (Grant No. SEV-2017-0706) and is funded by the CERCA Programme/Generalitat de Catalunya. 7. Recommended citation for this dataset: Liang, Zhifu; Wang, Jianghao; Tang, Peng-Yi; Tang, Weiqiang; Liu, Lijia; Shakouri, Mohsen; Wang, Xiang; Llorca, Jordi; Zhao, Shuangliang; Heggen, Marc; Dunin-Borkowski, Rafal E.; Cabot, Andreu; Wu, Hao Bin; Arbiol, Jordi; 2022; Supplementary material of the article Molecular Engineering to Introduce Carbonyl Between Nickel Salophen Active Sites to Enhance Electrochemical CO2 Reduction to Methanol [Dataset]; Elsevier; http://doi.org/10.1016/j.apcatb.2022.121451 SHARING/ACCESS/CONTEXT INFORMATION 1. Usage Licenses/restrictions placed on the data (please indicate if different data files have different usage license): https://creativecommons.org/licenses/by-nc-nd/4.0/ 2. Links to publications/other research outputs that cite the data: N/A 3. Links to publications/other research outputs that use the data: Liang, Zhifu; Wang, Jianghao; Tang, Peng-Yi; Tang, Weiqiang; Liu, Lijia; Shakouri, Mohsen; Wang, Xiang; Llorca, Jordi; Zhao, Shuangliang; Heggen, Marc; Dunin-Borkowski, Rafal E.; Cabot, Andreu; Wu, Hao Bin; Arbiol, Jordi. Molecular engineering to introduce carbonyl between nickel salophen active sites to enhance electrochemical CO2 reduction to methanol. http://doi.org/10.1016/j.apcatb.2022.121451. http://hdl.handle.net/10261/278989 4. Links to other publicly accessible locations of the data: N/A 5. Links/relationships to ancillary data sets: N/A 6. Was data derived from another source? If so, please add link where such work is located: N/A DATA & FILE OVERVIEW 1. File List: Supplementary_material_Molecular_Engineering.pdf 2. Relationship between files, if important: N/A 3. Additional related data collected that was not included in the current data package: N/A 4. Are there multiple versions of the dataset? If so, please indicate where they are located: N/A METHODOLOGICAL INFORMATION 1. Description of methods used for collection/generation of data: Figure S1. Synthesis scheme of Ni-2D-SA. -- Figure S2. PXRD patterns of Ni-2D-SA (black) and Ni-2D-O-SA (red). -- Figure S3. FT-IR spectra of Ni-2D-SA and Ni-2D-O-SA. -- Figure S4. chemical shift of 13C SSNMR spectra of Ni-2D-SA and Ni-2D-O-SA. -- Figure S5 SEM images of: (a) Ni-2D-O-SA, (b) Ni-2D-O-SA-CNT, (c) Ni-2D-SA-CNT. -- Figure S6. (a)-(c) HAADF-STEM images of Ni-2D-O-SA displaying the presence of atomically dispersed nickel atoms. (d) HAADF-STEM image and EDS mapping. -- Figure S7. Fourier transformed Ni K-edge EXAFS spectra of Ni-SA plotted in R-space, Fourier transformed EXAFS spectra in R-space of Ni-SA and fitted curve. -- Table S1. The Ni K-edge EXAFS fitting parameters of Ni-SA. R：bond length, CN: coordination number. -- Figure S8. Fourier transformed Ni K-edge EXAFS spectra of Ni-2D-SA plotted in R-space, Fourier transformed EXAFS spectra in R-space of Ni-SA and fitted curve. -- Table S2. The Ni K-edge EXAFS fitting parameters of Ni-2D-SA. -- Table S3. The Ni K-edge EXAFS fitting parameters of Ni-2D-O-SA. -- Figure S9. Fourier transformed Ni K-edge EXAFS spectra of Ni-2D-O-SA after immersed in KHCO3 for three days plotted in R-space, Fourier transformed EXAFS spectra in R-space of Ni-SA and fitted curve. -- Table S4. The Ni K-edge EXAFS fitting parameters of Ni-2D-O-SA-KHCO3. -- Figure S10. Pore size distribution of Ni-2D-SA and Ni-2D-O-SA powder, respectively. -- Figure S11. PXRD of Ni-2D-SA-CNT, Ni-2D-O-SA-CNT and CNT. -- Figure S12. HAADF-STEM image and EDS elemental mapping for Ni-2D-O-SA-CNT. -- Figure S13. Left panel: i-t curve on Ni-2D-O-SA-CNT at -0.9 V vs. RHE for 1h Right panel: Calibration curves for methanol (0.2 mM DMSO as internal standard). -- Figure S14. NMR spectrum of the catholyte after 1 hour of CO2 reduction on Ni-2D-O-SA-CNT. -- Figure S15. (a and b) Current densities of CO2RR for Ni-2D-O-SA-CNT and Ni-2D-SA-CNT at various potentials. (c and d) Product distribution of CO2RR for Ni-2D-O-SA-CNT and Ni-2D-SA-CNT at various potentials. -- Figure S16. (a,c) CV curves on Ni-2D-O-SA-CNT and Ni-2D-SA-CNT with different scan rates (5, 10, 20, 50, 100 mV s-1). (b, d) Current at open circuit potential (OCP) versus scan rates of different samples. The electrode area is 1 cm-2. -- Figure S17. Product distribution for Ni-2D-O-SA-CNT under Ar-saturated 0.1 M KHCO3 electrolyte at various potentials. -- Figure S18. NMR spectrum of the catholyte after 1 hour of CO2 reduction on Ni-2D-O-SA-CNT. -- Figure S19. NMR spectrum of the catholyte after 1 hour of electro-reduction under Ar environment on Ni-2D-O-SA-CNT. -- Figure S21. XPS spectra of Ni-2D-O-SA-CNT on carbon paper before and after 1 and 5 hours of CO2RR test. -- Figure S22. Product distribution of CO2RR for 2D-O-SA-CNT (without nickel) at various potential. -- Figure S23. Free-energy profiles of hydrogen evolution reaction (HER) on selected segments of Ni-2D-SA and Ni-2D-O-SA, respectively. -- Figure S24. The adsorption energy for intermediates (from CO to methanol) on selected segments of Ni-2D-SA and Ni-2D-O-SA, respectively. -- Figure S25. Free energy diagram of CO2 to CH3OH on selected segments of Ni-2D-O-SA. -- Table S5. Performance comparison of our catalysts and previous reported molecular based electrocatalysts for conversion of CO2 to methanol. 2. Methods for processing the data: N/A 3. Instrument- or software-specific information needed to interpret/reproduce the data, please indicate their location: N/A 4. Standards and calibration information, if appropriate: N/A 5. Environmental/experimental conditions: N/A 6. Describe any quality-assurance procedures performed on the data: N/A 7. People involved with sample collection, processing, analysis and/or submission, please specify using CREDIT roles https://credit.niso.org/: N/A 8. Author contact information: Wang, Jianghao [wjh7744@zju.edu.cn] Cabot, Andreu [acabot@irec.cat] Wu, Hao Bin [hbwu@zju.edu.cn] Arbiol, Jordi [arbiol@icrea.cat] DATA-SPECIFIC INFORMATION: 1. Number of variables: N/A 2. Number of cases/rows: N/A 3. Variable List: N/A 4. Missing data codes: N/A 5. Specialized formats or other abbreviations used: N/A 6. Dictionaries/codebooks used: N/A 7. Controlled vocabularies/ontologies used: N/A