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ARTICLE NATURE COMMUNICATIONS | https://doi.org/10.1038/s41467-020-20287-w components were bolted together with eight #10–24 bolts. A peristaltic pump (Cole-Parmer Masterflex L/S) was used to circulate the electrolytes between the electrolyte reservoirs (contained in 15 mL polypropylene centrifuge tubes) and the SFB/RFB cells via PharMed BPT tubing. RFB device characterizations. All RFB and SFB measurements were carried out in a custom modified N2 flush box (Terra Universal) with continuous N2 purging. 5.0 mL solution of 0.2 M BTMAP-Fc and 5.0 mL solution of 0.2 M BTMAP-Vi, both with 1.0 M NaCl as the supporting salt, were used as anolyte and catholyte, respectively. Both BTMAP-Fc and BTMAP-Vi were purchased from the Tokyo Chemical Industry Co., Ltd. and used directly. The NMe-TEMPO was synthesized following a previous report50. The electrolyte flow rate was set from 20 to 120 mL min−1 for RFB mea- surements. Galvanostatic cycling tests were carried out using a Bio-Logic BP-300 potentiostat at desired constant current densities with 0.3 and 1.1 V as the bottom and top potential limits, respectively. A 10 s rest period at open-circuit voltage was employed between each half cycle. The potentiostatic capacity of the RFB was determined by galvanostatic charging/discharging followed by a potential hold at cut- off potentials until the current density reached 1 mA cm−2. SFB device characterizations. Totally, 5.0 mL solution of BTMAP-Vi/Fc with concentrations of 0.1 and 0.2 M in 1.0 M NaCl, or 5.0 mL solution of BTMAP-Fc/ NMe-TEMPO with concentrations of 0.1 M in 1.0 M NaCl were used as the cath- olyte/anolyte. The electrolyte flow rate was controlled at 40, 60, and 80 mL min−1 for the SFB cycling tests. A dual-channel Bio-Logic BP-300 potentiostat was used for the SFB cycling tests. To characterize the charging–discharging behaviors of the integrated SFB device, one potentiostat channel (CH1) was configured as the RFB mode to monitor the potential between the two carbon felt electrodes; the other potentiostat channel (CH2) was configured as solar recharge mode to monitor the charging photocurrent (Fig. 1c). During the solar charging process, the GaAs photoelectrode was illuminated by one Sun simulation (as described in the PEC characterization section) without applying external bias. A 1.35 h time limit was used to control the SOC below ca. 54%. During the discharging process, the illumination was blocked by a beam shutter, and a discharging current intensity of 11 mA was applied by CH1 until the cell potential reached 0.3 V. The dual-channel potentiostat and the beam shutter of the solar simulator were synchronized and controlled by CH1 and a custom-made electronic control box to enable automated long-term SFB cycling measurements. Potential match calculation and simulations. To optimize the potential match Data availability All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Information. Additional data related to this paper may be requested from the corresponding authors upon reasonable request. Source data are provided with this paper. Received: 8 July 2020; Accepted: 16 November 2020; References 1. Lewis, N. S. Research opportunities to advance solar energy utilization. Science 351, aad1920 (2016). 2. Walter, M. G. et al. Solar water splitting cells. Chem. Rev. 110, 6446–6473 (2010). 3. Gurung, A. & Qiao, Q. Solar charging batteries: advances, challenges, and opportunities. Joule 2, 1217–1230 (2018). 4. Zeng, Q. et al. Integrated photorechargeable energy storage system: next generation power source driving the future. Adv. Energy Mater. 10, 1903930 (2020). 5. Shaner, M. R., Atwater, H. A., Lewis, N. S. & McFarland, E. W. 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Note 0 cell cell that Ecell generally remains constant with given anolyte/catholyte combination, but the actual cell potential of SFB (Ecell) changes with SOC and needs to be calculated by the Nernst equation: E 1⁄4 E0 RT ln1SOC2 þIR ; ð5Þ cell cell nF SOC DC where R is the universal gas constant, T is temperature, n is the number of electrons transferred in a redox reaction, F is Faraday constant, I is the applied current, and RDC is the DC series resistance of SFB under RFB mode64. The solar conversion efficiency of SFBs at specific SOCs was quantitatively assessed by SOEEins (Eq. 4). The equations for calculating the CE, VE, and EE are CE 1⁄4 Qdischarge 1⁄4 R Qcharge R Iout dt ; Ioperating dt dt ð6Þ ð7Þ ð8Þ R VE 1⁄4 Vdiscahrge 1⁄4 R dt " V" cahrge V R dt ; EE 1⁄4 Edischarge ; Echarge where Iout is the discharging current and Vout is the cell potential extracted from data during the discharging process. Therefore, the qualitative relationship between SOEEins and Ecell (or SOC) at specific E0cell can be obtained (Fig. 3b, Supplementary Fig. 11, and Supplementary Fig. 12). The overall SOEE of SFB charged in a specific SOC range (x to y, usually from 1% to 99% if not specified otherwise) was then calculated as the integral average of SOEEins with respect to SOC. Ry SOEE1⁄4 x SOEE ðSOCÞdSOC : R ins ð9Þ y x dSOC V dt Rout operating By repeating the calculation described above with different E0cell and a 10 mV interval, the qualitative relationship between SOEE and E0cell can be obtained (Figs. 1d and 5a and Supplementary Fig. 14). 10 NATURE COMMUNICATIONS | (2021)12:156 | https://doi.org/10.1038/s41467-020-20287-w | www.nature.com/naturecommunicationsPDF Image | flow battery enabled single-junction GaAs photoelectrode
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