Hydrogen Peroxide Generation with 100% Faradaic Efficiency on Metal-Free Carbon Black

Wang, Zhe; Li, Qin-Kun; Zhang, Chenhao; Cheng, Zhihua; Chen, Wei-Yin; McHugh, Emily A.; Carter, Robert A.; Yakobson, Boris I.; Tour, James M.

doi:10.1021/acscatal.0c04735

Cited by 129 publications

(103 citation statements)

References 59 publications

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“…[23][24][25][26][27][28][29][30][31][32][33][34][35] Wherein, the oxygen-doped carbon catalysts have gained the special attentions because of their high H 2 O 2 selectivity during ORR. [36][37][38][39][40][41][42] For example,D ong et al [42] reported that the superhydrophilic honeycomb carbon nanofiber with rich oxygenated functional groups showed high H 2 O 2 selectivity during ORR. In this community,r esearchers focus on developing highly efficient catalyst and identifying the active sites for 2e À ORR.…”

Section: Introductionmentioning

confidence: 99%

Chemical Identification of Catalytically Active Sites on Oxygen‐doped Carbon Nanosheet to Decipher the High Activity for Electro‐synthesis Hydrogen Peroxide

et al. 2021

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Electrochemical production of hydrogen peroxide (H 2 O 2 )t hrough two-electron (2 e À )o xygen reduction reaction (ORR) is an on-site and clean route.O xygen-doped carbon materials with high ORR activity and H 2 O 2 selectivity have been considered as the promising catalysts,h owever,t here is still alackofdirect experimental evidence to identify true active sites at the complex carbon surface.H erein, we propose ac hemicalt itration strategy to decipher the oxygen-doped carbon nanosheet (OCNS 900 )c atalyst for 2e À ORR. The OCNS 900 exhibits outstanding 2e À ORR performances with onset potential of 0.825 V( vs.R HE), mass activity of 14.5 Ag À1 at 0.75 V( vs.R HE) and H 2 O 2 production rate of 770 mmol g À1 h À1 in flow cell, surpassing most reported carbon catalysts.Through selective chemical titration of C = O, C À OH, and COOH groups,wefound that C = Ospecies contributed to the most electrocatalytic activity and were the most active sites for 2e À ORR, which were corroborated by theoretical calculations.

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Section: Introductionmentioning

confidence: 99%

Chemical Identification of Catalytically Active Sites on Oxygen‐doped Carbon Nanosheet to Decipher the High Activity for Electro‐synthesis Hydrogen Peroxide

et al. 2021

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“…Analogously, SW defect is further depicted in Figure 4d1, which is reconstructed from four hexagonal carbon rings. Moreover, theoretical and experimental studies suggest that the carbon atoms simultaneously linked by 5-7 rings in SW defects are active sites to facilitate the ORHP 7 .…”

Section: Resultsmentioning

confidence: 99%

“…Chiefly, oxidized carbon materials (such as oxidized carbon black 7 , oxidized CNTs 8 , oxygenated graphitic nanoplatelets 9 ) have emerged as a type of promising catalyst for ORHP, due to the oxygen moieties improving the OOH* absorption capacity of the adjacent carbon atoms. Nevertheless, oxidized carbon materials generally suffer from surface oxidization at high current, showing sluggish kinetics.…”

Section: Introductionmentioning

confidence: 99%

Marginal defects modified graphene with S-C-N-C groups for highly selective oxygen reduction to H2O2

Mou¹,

Mu²,

Liu³

et al. 2021

Preprint

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Developing efficient metal-free catalysts to achieve electrochemical synthesis of hydrogen peroxide (H2O2) is crucial for substituting traditional energy-intensive anthraquinone process. Heteroatom-doped carbon materials have shown great potential toward 2e-pathway for catalyzing oxygen reduction to hydrogen peroxide (ORHP). However, conventional nanocarbon electrocatalysts show slow kinetics toward ORHP due to the weak binding strength with OOH* intermediate, resulting reduction of O2 to H2O. Here, sulfur and nitrogen dual-doped graphene (SNC) electrocatalyst consisting of S-C-N-C functional group are synthesized through hydrothermal self-assembly and nitridation processes with thiourea as sulfur source. In S-C-N-C functional group, pentagon-S and pyrrolic-N are covalently grafted onto the edge of graphene and produce marginal carbon ring defects, which provide highly active sites for catalyzing ORHP. The obtained SNC catalysts deliver an outstanding ORHP activity and selectivity for H2O2 production, while retaining remarkable stability. The experimental and computational results reveal that marginal S-C-N-C functional groups afford an appropriate adsorption strength with OOH* intermediate and a low reaction barrier as well, which are essential for the activity of ORHP.

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“…[ 14 ] However, recent work indicated that the carbon defects generated during the oxidation process also play an important role. [ 71 ] Effects may be more complicated in N‐doped and other heteroatom‐doped materials. Further exploration can help understand the catalytic process and design better catalysts.…”

Section: Discussionmentioning

confidence: 99%

Metal‐Free Electrocatalysts for Oxygen Reduction to Hydrogen Peroxide

Wang

James

Tour

2021

Adv Energy and Sustain Res

Self Cite

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Hydrogen peroxide (H 2 O 2 ), as an environmentally friendly and highly efficient oxidation reagent, is now widely and increasingly used in many areas. The traditional anthraquinone synthesis process, however, is energy and capital intensive with low efficiency. Electrochemically reducing oxygen (O 2 ) to H 2 O 2 with metal-free catalysts is considered a promising alternative. This work describes the two-electron oxygen reduction process from both thermodynamic and kinetic aspects and summarizes the designing rules for effective H 2 O 2 formation catalysts. This includes tuning the binding energy of the intermediate species, the concentration of dissociation active sites, and adjusting the dielectric constant of solvents. These principles are successfully applied to the design of various metal-free catalysts by proper structure engineering and heteroatom doping, which shows both high activity and efficiency. Furthermore, pH and temperature effects are presented with a view toward reaction optimization. An outlook of future challenges is also discussed.

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Hydrogen Peroxide Generation with 100% Faradaic Efficiency on Metal-Free Carbon Black

Cited by 129 publications

References 59 publications

Chemical Identification of Catalytically Active Sites on Oxygen‐doped Carbon Nanosheet to Decipher the High Activity for Electro‐synthesis Hydrogen Peroxide

Chemical Identification of Catalytically Active Sites on Oxygen‐doped Carbon Nanosheet to Decipher the High Activity for Electro‐synthesis Hydrogen Peroxide

Marginal defects modified graphene with S-C-N-C groups for highly selective oxygen reduction to H2O2

Metal‐Free Electrocatalysts for Oxygen Reduction to Hydrogen Peroxide

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