Chinese Journal of Catalysis ›› 2021, Vol. 42 ›› Issue (12): 2149-2163.DOI: 10.1016/S1872-2067(20)63781-0
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Received:
2021-01-06
Accepted:
2021-01-06
Online:
2021-12-18
Published:
2021-05-06
Contact:
Gang Wu
About author:
* Tel: +1-716-6458618; Fax: +1-716-6453822; E-mail: gangwu@buffalo.eduYachao Zeng, Gang Wu. Electrocatalytic H2O2 generation for disinfection[J]. Chinese Journal of Catalysis, 2021, 42(12): 2149-2163.
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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(20)63781-0
Fig. 1. Destruction of infectious agents by ROS. The susceptibility to oxidative damages can be ordered as viruses > prions > Gram (-) bacteria > Gram (+) bacteria > yeasts > molds. ROS will eventually oxidize organic matter and dead microbial cells into CO2 and H2O. Reproduced with permission [35]. Copyright 2015, Springer.
Fig. 3. Electrochemical H2O2 generation via the ORR, the WOR and the association pathways with the transient intermediates on the different catalyst surfaces.
Fig. 4. (a) A schematic illustrating the possible reaction pathway steered by local concentrate O2. (b) Optical image for PTFE-patterned glassy carbon (GC) at 2.05 VRHE in 1.0 M Na2CO3 electrolyte. (c) Adhesive force measurements of O2 gas bubble on pristine GC, 300-GC and 200-GC electrodes, demonstrating enhanced O2 adhesive force of the GC surface by PTFE coating. (d) Comparison of total current densities in the pristine carbon fiber paper (CFP), CFP-5%, CFP-20% and CFP-60% catalysts. (e) The FE of pristine GC, 300-GC and 200-GC catalysts at 2.05 VRHE in 1.0 M Na2CO3 electrolyte. (f) A comparison of H2O2 generation rates of CFP-60% catalyst against other catalyst systems under different applied potentials. Reproduced with permission [92]. Copyright 2020, Springer Nature.
Fig. 5. (a) A general synthetic strategy for platinoid SACs; HAADF-STEM image (b) and Pt L3-edge k3-weighted EXAFS spectrum and the best fit (c) for 3Pt/CNT_IL_SiO2; (d) ORR activity and selectivity of 3Pt/CNT_IL_SiO2 in 0.1 M HClO4; (e) A comparison of H2O2 yields in nanoparticle and single atom catalysts at -0.5 mA cm-2, in which M/CNT and M/CNT_IL_SiO2 are denoted as MNP and M1, respectively; (f) Linear relationship between the DFT-calculated ΔGO values and the experimentally determined H2O2 yields of the SACs; (g) Volcano plot between the O binding energies and the onset potentials for the 2e- ORR pathway for SACs and NP catalysts. Reproduced with permission [127]. Copyright 2020, American Society of Chemistry.
Fig. 6. (a) Schematic illustration of various M-N-C SACs (M = Mn, Fe, Co, Ni, Cu) and their preferred ORR pathways. (b) Correlation of binding energy of *OOH, *O, and *OH on M-SAC (M = Mn, Fe, Co, Ni, and Cu) and d-bond center (open circle) of M atom in M-SAC (M = Mn, Fe, Co, Ni, and Cu). Reprinted with permission [118]. Copyright 2020, Elsevier Inc. (c) H2O2 production current as a function of the binding energy of OH* intermediate. (d) H2O2 selectivity (H2O2 %) and the electrons transfer number (n) at 0.1 VRHE over various M-N-C SACs. Reproduced with permission [119]. Copyright 2019, American Society of Chemistry. Comparison of H2O2 selectivity (e) and H2O2 current at 0.7 V (f) for NG(O), Co1-NG(O) and Co1-NG(R). (g) ORR volcano plots for the production of H2O (blue) and H2O2 (red). Red and blue data points are Co-N4/graphene catalyst with electron-rich species (O*/2O*) and electron-poor species (4H*/2H*) adsorbed close to the cobalt atom, respectively. Reproduced with permission [128]. Copyright 2020 Springer Nature.
Fig. 7. (a) Reconstructed atom probe tomography of Fe-CNT catalyst. TEM (b), HAADF-STEM (c) and XAS (d) characterizations of Fe-CNT catalyst. (e) Overall ORR current and (f) corresponding H2O2 selectivity of Fe-, Pd-, Co-, Mn-CNT catalysts. (g) Schematic illustration of electrochemical H2O2 generation for water disinfection, powering with renewable energy. (h) The disinfection efficacy as a function of reaction time. Reprinted with permission from Ref. [117]. Copyright 2019, Nature Publishing Group.
Fig. 8. (a) Schematic illustrations of the NADE fabrication process and the three-phase electrocatalytic system; In-panel (b) and cross-sectional (c) SEM images of modified carbon felt with contact angle (inset); (d) The concentration profiles of H2O2 production in different systems at 60 mA cm-2 current density. Reproduced with permission [147]. Copyright 2020, Springer Nature.
Fig. 9. (a) Schematic diagram of the H2O2 generation in a membrane-free electrolyzer mode. Reprinted with permission [153]. Copyright 2017, The Royal Society of Chemistry. (b) Membrane-based flow reactor containing a MEA. The MEA is sandwiched between the anode and cathode current collectors with flow field patterns. Reprinted with permission [27]. Copyright 2020, American Society of Chemistry. (c) Electrochemical H2O2 generation by using pure H2 and O2 streams separately introduced to the anode and cathode. SE denotes a solid electrolyte, which consisted of either functionalized styrene-divinylbenzene copolymer microspheres or inorganic CsxH3?xPW12O40 in this study. Electrochemically produced H+ and HO2-, driven by the electric field, cross in the porous SE layer and form H2O2. H2O2 with no impurities is carried out by flowing DI water through the porous SE layer. Reprinted with permission [154]. Copyright 2019, AAAS. (d) Illustration of overall phase-transfer strategy for electrochemical H2O2 generation. Reproduced with permission [155]. Copyright 2019, Elsevier Inc.
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