Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media
Electrochemical hydrogen peroxide (H2O2) production (EHPP) via a two-electron oxygen reduction reaction (2e- ORR) provides a promising alternative to replace the energy-intensive anthraquinone process. M-N-C electrocatalysts, which consist of atomically dispersed transition metals and nitrogen-doped...
| Main Authors: | , , , , , , , , , , , , , , , , , , , , , , |
|---|---|
| Format: | Journal article |
| Language: | English |
| Published: |
Nature Research
2024
|
| _version_ | 1826313604689821696 |
|---|---|
| author | Liu, L Kang, L Feng, J Hopkinson, DG Allen, CS Tan, Y Gu, H Mikulska, I Celorrio, V Gianolio, D Wang, T Zhang, L Li, K Zhang, J Zhu, J Held, G Ferrer, P Grinter, D Callison, J Wilding, M Chen, S Parkin, I He, G |
| author_facet | Liu, L Kang, L Feng, J Hopkinson, DG Allen, CS Tan, Y Gu, H Mikulska, I Celorrio, V Gianolio, D Wang, T Zhang, L Li, K Zhang, J Zhu, J Held, G Ferrer, P Grinter, D Callison, J Wilding, M Chen, S Parkin, I He, G |
| author_sort | Liu, L |
| collection | OXFORD |
| description | Electrochemical hydrogen peroxide (H2O2) production (EHPP) via a two-electron oxygen reduction reaction (2e- ORR) provides a promising alternative to replace the energy-intensive anthraquinone process. M-N-C electrocatalysts, which consist of atomically dispersed transition metals and nitrogen-doped carbon, have demonstrated considerable EHPP efficiency. However, their full potential, particularly regarding the correlation between structural configurations and performances in neutral media, remains underexplored. Herein, a series of ultralow metal-loading M-N-C electrocatalysts are synthesized and investigated for the EHPP process in the neutral electrolyte. CoNCB material with the asymmetric Co-C/N/O configuration exhibits the highest EHPP activity and selectivity among various as-prepared M-N-C electrocatalyst, with an outstanding mass activity (6.1 × 105 A gCo−1 at 0.5 V vs. RHE), and a high practical H2O2 production rate (4.72 mol gcatalyst−1 h−1 cm−2). Compared with the popularly recognized square-planar symmetric Co-N4 configuration, the superiority of asymmetric Co-C/N/O configurations is elucidated by X-ray absorption fine structure spectroscopy analysis and computational studies. |
| first_indexed | 2024-09-25T04:17:33Z |
| format | Journal article |
| id | oxford-uuid:a18c4016-102b-49d1-b6cf-4a93a1e065f6 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-09-25T04:17:33Z |
| publishDate | 2024 |
| publisher | Nature Research |
| record_format | dspace |
| spelling | oxford-uuid:a18c4016-102b-49d1-b6cf-4a93a1e065f62024-07-20T15:59:21ZAtomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral mediaJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:a18c4016-102b-49d1-b6cf-4a93a1e065f6EnglishJisc Publications RouterNature Research2024Liu, LKang, LFeng, JHopkinson, DGAllen, CSTan, YGu, HMikulska, ICelorrio, VGianolio, DWang, TZhang, LLi, KZhang, JZhu, JHeld, GFerrer, PGrinter, DCallison, JWilding, MChen, SParkin, IHe, GElectrochemical hydrogen peroxide (H2O2) production (EHPP) via a two-electron oxygen reduction reaction (2e- ORR) provides a promising alternative to replace the energy-intensive anthraquinone process. M-N-C electrocatalysts, which consist of atomically dispersed transition metals and nitrogen-doped carbon, have demonstrated considerable EHPP efficiency. However, their full potential, particularly regarding the correlation between structural configurations and performances in neutral media, remains underexplored. Herein, a series of ultralow metal-loading M-N-C electrocatalysts are synthesized and investigated for the EHPP process in the neutral electrolyte. CoNCB material with the asymmetric Co-C/N/O configuration exhibits the highest EHPP activity and selectivity among various as-prepared M-N-C electrocatalyst, with an outstanding mass activity (6.1 × 105 A gCo−1 at 0.5 V vs. RHE), and a high practical H2O2 production rate (4.72 mol gcatalyst−1 h−1 cm−2). Compared with the popularly recognized square-planar symmetric Co-N4 configuration, the superiority of asymmetric Co-C/N/O configurations is elucidated by X-ray absorption fine structure spectroscopy analysis and computational studies. |
| spellingShingle | Liu, L Kang, L Feng, J Hopkinson, DG Allen, CS Tan, Y Gu, H Mikulska, I Celorrio, V Gianolio, D Wang, T Zhang, L Li, K Zhang, J Zhu, J Held, G Ferrer, P Grinter, D Callison, J Wilding, M Chen, S Parkin, I He, G Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media |
| title | Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media |
| title_full | Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media |
| title_fullStr | Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media |
| title_full_unstemmed | Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media |
| title_short | Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media |
| title_sort | atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media |
| work_keys_str_mv | AT liul atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT kangl atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT fengj atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT hopkinsondg atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT allencs atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT tany atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT guh atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT mikulskai atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT celorriov atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT gianoliod atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT wangt atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT zhangl atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT lik atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT zhangj atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT zhuj atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT heldg atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT ferrerp atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT grinterd atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT callisonj atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT wildingm atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT chens atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT parkini atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia AT heg atomicallydispersedasymmetriccobaltelectrocatalystforefficienthydrogenperoxideproductioninneutralmedia |