<p>Eco-friendly electrocatalytic production of alkaline H<sub>2</sub>O<sub>2</sub> via the two-electron oxygen reduction reaction offers a promising alternative to the conventional anthraquinone process, which is energy-intensive and poses explosion risks. However, the industrial adoption of this approach is hindered by sluggish proton-feeding kinetics of heterogeneous electrocatalysts, which restricts the achievable current densities. Herein, we develop Ni-based metal-organic frameworks with a bio-inspired B-coordination (B-NiBDC). The B-NiBDC shows Faradaic efficiency of ~90% for H<sub>2</sub>O<sub>2</sub> electrosynthesis at 1000 mA cm<sup>−2</sup>, obtaining ~7.49 wt.% H<sub>2</sub>O<sub>2</sub> alkaline solution for bleaching under urea oxidation-assisted energy-saving system. This has led to a significant increase in pulp brightness by 25-39 % (International Organization for Standardization, ISO). We propose that B-O-Ni motifs of B-NiBDC induce the formation of electron-deficient Ni active sites. Experiments and theoretical calculations elucidate that the electron-deficient Ni has accelerated water dissociation kinetics for proton-feeding to produce *OOH intermediate with suitable adsorption energy, boosting overall H<sub>2</sub>O<sub>2</sub> electrosynthesis activity.</p>

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Enhanced proton-feeding kinetics of metal-organic framework toward industrial-level H2O2 electrosynthesis for sustainable bleaching

  • Fanpeng Cheng,
  • Yingnan Liu,
  • Zilin Zhao,
  • Xiaoxuan Yang,
  • Wanzhen Zheng,
  • Bin Yang,
  • Zhongjian Li,
  • Qinghua Zhang,
  • Chung-Li Dong,
  • Lecheng Lei,
  • Liming Dai,
  • Yang Hou

摘要

Eco-friendly electrocatalytic production of alkaline H2O2 via the two-electron oxygen reduction reaction offers a promising alternative to the conventional anthraquinone process, which is energy-intensive and poses explosion risks. However, the industrial adoption of this approach is hindered by sluggish proton-feeding kinetics of heterogeneous electrocatalysts, which restricts the achievable current densities. Herein, we develop Ni-based metal-organic frameworks with a bio-inspired B-coordination (B-NiBDC). The B-NiBDC shows Faradaic efficiency of ~90% for H2O2 electrosynthesis at 1000 mA cm−2, obtaining ~7.49 wt.% H2O2 alkaline solution for bleaching under urea oxidation-assisted energy-saving system. This has led to a significant increase in pulp brightness by 25-39 % (International Organization for Standardization, ISO). We propose that B-O-Ni motifs of B-NiBDC induce the formation of electron-deficient Ni active sites. Experiments and theoretical calculations elucidate that the electron-deficient Ni has accelerated water dissociation kinetics for proton-feeding to produce *OOH intermediate with suitable adsorption energy, boosting overall H2O2 electrosynthesis activity.