Supplementary Information

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1 Supplementary Information Cooperative cathode electrode and in situ deposited copper for subsequent enhanced Cd(II) removal and hydrogen evolution in bioelectrochemical systems Qiang Wang 1, Liping Huang 1,*, Yuzhen Pan 2, Peng Zhou 2, Xie Quan 1,*, Bruce E. Logan 3, 6 Hongbo Chen Key Laboratory of Industrial Ecology and Environmental Engineering, Ministry of 9 Education (MOE), School of Environmental Science and Technology, Dalian University of 10 Technology, Dalian , China College of Chemistry, Dalian University of Technology, Dalian , China Department of Civil and Environmental Engineering, The Pennsylvania State University, 13 University Park, Pennsylvania, Corresponding authors: 16 (Huang L.) lipinghuang@dlut.edu.cn, Tel./Fax.: (Quan X.) quanxie@dlut.edu.cn, Tel.: Page: 10 Figure: 4 Table: 3 1

2 Fig. S1 Schematic diagram of BESs at MFC or MEC mode through a time electromagnetic relay

3 Fig. S2 Sketch map of competitive relationships between Cd(II) reduction and hydrogen evolution, and ratios of charges for Cd(II) reduction and hydrogen evolution on the different material cathodes of TS, NF and CC. 49 3

4 Fig. S3 Comparison of (A) Cd(II) removal rates, (B) hydrogen production, and (C) current densities on the various material cathodes with deposited copper in the catholytes of CdCl 2 or CdSO 4 (applied voltage: 0.5 V, deposited copper: 150 mg/l)

5 Fig. S4 (A) Cd(II) removal rates, (B) hydrogen production, (C) current densities, and (D) cathode and anode potentials as a function of applied voltage in MEC mode and with various material cathodes (copper deposited using a solution of 150 mg/l)

6 Fig. S5 (A) Cd(II) removal rates, (B) hydrogen production and (C) current densities as a function of number of batch cycles with fresh Cd(II) catholyte. Comparison of LSVs for the cathodes made of (D) TS, (E) NF and (F) CC with or without deposited copper, and after cycle 8 with fresh Cd(II) catholyte (deposited copper: 150 mg/l, applied voltage: 0.5 V, catholyte: CdSO 4 )

7 84 85 Table S1 Summary of the present studies applying BESs for Cu(II) and Cd(II) recovery, the processing parameters used, and the relevant recovery efficiency obtained. Applied voltage Operatio Final Initial metal or cathode BESs Reactor Cathode concentration Initial ph n time product Energy production Removal rate Ref. potential (mg/l) (h) (kwh/kg metal) (mg/l-h) (V vs SHE) Electron acceptor Cu(II) MFCs Dual chamber graphite foil Cu Heijne et al MFCs Dual chamber graphite rod Cu Cheng et al., 2013 MFCs Dual chamber graphite disk Cu Tao et al. 2011a MFCs Dual chamber graphite plate Cu Tao et al. 2011b MFCs Dual chamber graphite plate Cu Tao et al., 2011c MFCs Dual chamber graphite plate Cu(II)-a Zhang et al., mmonia 2012 MFCs Dual chamber graphite plate Cu Tao et al., 2014 MFCs Dual chamber graphite plate Cu An et al., 2014 MFCs Dual chamber TS Cu This study NF CC Cd(II) MFCs Single Abourached et Pt/CC NA CdS chamber al., 2014 MECs Dual chamber Titanium Modin et al., Cd wire 2012 MECs Dual chamber CC Cd Choi et al., 2014 MECs Dual chamber TS Cd Zhang et al., 2015 MECs Dual chamber TS Cd This study 7

8 86 87 TS + Cu NF NF + Cu CC CC + Cu

9 Table S2 Charge distribution, energy efficiency and overall energy recovery for Cd(II) reduction on the cathodes with different amounts of deposited copper (applied voltage: 0.5 V) Cu(II) Net charge η Electrode E η E+S concentration material (mg/l) Cd (C) H 2 (C) Cd(C)/H 2 (C) (X/Y) η E,Cd (%) η E,H2 (%) η E+S,Cd (%) η E+S,H2 (%) none 0.5 ± ± ± ± 3 90 ± 19 1 ± 0 7 ± ± ± ± ± ± 58 2 ± 0 13 ± 5 TS ± ± ± ± ± 43 2 ± 0 34 ± ± ± ± ± ± 4 2 ± 0 22 ± ± ± ± ± ± 13 1 ± 0 21 ± NF CC none 0.2 ± ± ± ± ± 4 0 ± 0 65 ± ± ± ± ± ± 7 1 ± 0 92 ± ± ± ± ± ± 6 1 ± ± ± ± ± ± ± 40 1 ± ± ± ± ± ± ± 8 1 ± 0 75 ± 3 none 0.6 ± ± ± ± ± 54 1 ± 0 13 ± ± ± ± ± ± 49 2 ± 0 33 ± ± ± ± ± ± 26 2 ± 0 62 ± ± ± ± ± ± 17 2 ± 0 58 ± ± ± ± ± ± 37 1 ± 0 53 ± 3 9

10 112 Table S3 Energy consumption for Cd(II) reduction and hydrogen evolution at various applied voltages (150 mg/l). Applied Parameter Electric energy Net electric energy Cathode voltage Net charge η E η E+S consumption consumption (V) Cd (C) H 2 (C) η E, Cd (%) η E, H2 (%) η E+S, Cd (%) η E+S, H2 (%) (kwh/kg Cd) (kwh/kg Cd) ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± 0.0 TS ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± NF CC ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ± ±

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