READ ME File For 'Dataset for Facilitating charge reactions in Al-S batteries with redox mediators' Dataset DOI: 10.5258/SOTON/D1848 ReadMe Author: John Lampkin, University of Southampton This dataset supports the publication: AUTHORS: He Li, John Lampkin, Nuria Garcia-Araez TITLE: Facilitating charge reactions in Al-S batteries with redox mediators JOURNAL: ChemSusChem PAPER DOI: 10.1002/cssc.202100973 This dataset contains: The figures are as follows: Figure 2: Voltage profile of unmediated and mediated Al-S cells in the first discharge/charge cycle with Uralumina electrolyte. The electrolytes were prepared by partially replacing the AlCl3 in the base Uralumina electrolyte (series 1, see Table 1). Experiments used a specific current of 50 mA gS-1 and the voltage range is 0.05-1.85 V. The sulfur loading in the electrodes was 1.3-1.9 mg cm-2. Figure 3: As in Figure 2 but with electrolytes prepared by partially replacing the urea in the base Uralumina by the mediator (series 2, Table 1). The sulfur loading in the electrodes was 1-1.1 mg cm-2. The differences in capacity with respect to the results in Figure 2 are due to the difference in sulfur loading, as shown in Figure 5. Figure 4: Voltage profile of Al-S cells with Uralumina electrolyte with 2.3 wt.% LiI mediator (series 1, see Table 1), obtained by charging the cells before discharge (solid black curves, inset shows a zoom-in). The voltage profile obtained with the standard protocol, with discharge prior to charge, is also shown for comparison (dashed red curves). All conditions as in Figure 2. The sulfur loading of charged first is 1.36 mg cm-2 and discharge first is 1.48 mg cm-2. Figure 5: Comparison of key performance parameters of Al-S batteries in Uralumina electrolyte with and without redox mediators, for the first discharge and charge cycle. The black points are the results with the bare Uralumina, and the red and blue points are with iodide or bromide mediators, respectively. The average discharge and charge voltage values are calculated using equation S2. Figure 6: Voltage profile of unmediated and mediated Al-S cells in the first discharge/charge cycle with [EMIM]Cl-AlCl3 (A,B,C) and [BMP]Cl-AlCl3 (D,E,F) electrolytes. Experiments used a specific current of 50 mA gS-1 and the voltage range is 0.05-1.85 V. The sulfur loading in the electrodes was 0.9-1.4 mg cm-2 for [EMIM]Cl containing cells and 0.9-1.6 mg cm-2 for [BMP]Cl containing cells. Figure 7: XRD pattern (grazing incidence, incident angle of 5°) of a sulfur cathode in the pristine form (blue), after discharge (black), and after charge (red) in an Al-S cell with 2.3 wt.% NaBr in [EMIM]Cl-AlCl3 electrolyte, using a specific current of 50 mA g-1. The pattern obtained with the XRD sample holder is also included (green). The sulfur peak positions are below (yellow) PDF No. 85-0799. Figure S2: Comparison of key performance parameters of Al-S batteries in Uralumina electrolyte with and without redox mediators. For series 1 data points, filled symbols are cells with 0.8 wt.% of mediators and non-filled symbols are 2.3 wt.% of mediator. Figure S3: Voltage profiles of Al-S cells with Uralumina electrolyte with different concentrations of redox mediators, as indicated, in the first (solid lines) and second (dashed lines) discharge/charge cycles. The electrolytes were prepared by partially replacing the AlCl3 in the base Uralumina electrolyte (series 1, see table 1). Experiments used a specific current of 50 mA gS-1 and the voltage range is 0.05-1.85 V. The sulfur loading in the electrodes was 1.3-1.8 mg cm-2. Figure S4: Evolution of the discharge capacity with cycle number (left) and Efficiency with cycle number (right) for Al-S cells with Uralumina electrolyte with different concentrations of redox mediators: A+B) 0.8 % and C+D) 2.3 % mediator (series 1, mediator partially replacing AlCl3), and E+F) 0.7 % mediator (series 2, mediator partially replacing urea). The sulfur loading in the electrodes was 1.3-1.9 mg cm-2 (Figure S4A&B), 1.3-1.8 mg cm-2 (Figure S4C&D) and 1.0-1.7 mg cm-2 (Figure S4E&F) respectively. Figure S5: Voltage profiles of Al-S cells in the first three cycles in A) Uralumina with 2.3 wt.% LiI and B) [EMIM]Cl-AlCl3 with of 2.3 wt.% LiI, showing an enlarged inset image displaying the additional voltage plateau that appears on the second discharge. Experiment used a specific current of 50 mA gS-1 and the voltage range is 0.05-1.85 V. The sulfur loading in the electrodes was: A) 1.48 and B) 0.99 mg cm-2. Figure S6: Comparison of key performance parameters of Al-S batteries in [EMIM]Cl-AlCl3 electrolyte with and without redox mediators. 1 and 2.3 wt.% mediator solutions correspond to filled and non-filled data points respectively. In the charge capacity plot, the cells with Iodide redox mediator exceeded the time 60 hour cut-off limit, and hence the capacity values plotted equal the capacity limit of 3000 mAh g-1 set in the measurements. Figure S8: Voltage profile of Al-S cells with [EMIM]Cl-AlCl3 electrolyte with 2.3 wt.% LiI mediator (series 1, see Table 1), obtained by charging the cells before discharge (solid black curves, inset shows a zoom-in). The voltage profile obtained with the standard protocol, with discharge prior to charge, is also shown for comparison (dashed red curves). Experiments used a specific current of 50 mA gS-1 and the voltage range is 0.05-1.85 V. The sulfur loading of charged first is 1.11 mg cm-2 and discharge first is 0.99 mg cm-2. Date of data collection: 12/08/2019 to 02/12/2020 Information about geographic location of data collection: Southampton, UK Licence: CC-BY Related projects: European Commission Horizon 2020 FEP-OPEN project SALBAGE (766581), EPSRC (EP/N024303/1) Date that the file was created: June, 2021