Host-guest-induced electronic state triggers two-electron oxygen reduction electrocatalysis

Chen, Hongni; Wang, Chao; Wu, Han; Li, Lili; Xing, Yali; Zhang, Chuanhui; Long, Xiaojing

doi:10.1038/s41467-024-53714-3

Nat Commun

2024

DOI: 10.1038/s41467-024-53714-3

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Host-guest-induced electronic state triggers two-electron oxygen reduction electrocatalysis

Hongni Chen,

Chao Wang,

Han Wu

et al.

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Cited by 5 publications

References 65 publications

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Electron‐Deficient Organic Molecules Based on B←N Unit: A N‐Type Room‐Temperature Chemiresistive Sensors with Moisture Resistance

Wang,

Xing,

Zhang

et al. 2024

Advanced Science

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Organic molecules with tailorable chemical structures, high stability, and solution processability have great potential in the sensing field. Compared with p‐type organic small molecules (OSMs), the electron‐dominated n‐type analogs show superior conductivity when exposed to reducing gases, which can achieve outstanding sensor signal‐to‐noise ratios. However, inadequate humidity resistance at room temperature hinders the development of such molecules. Herein, an A‐D‐π‐D‐A molecular design strategy is proposed based on electron‐deficient B←N units, which results in effective intramolecular charge transport and sensitive responses by extending the π‐conjugation bridge. As a result, the ST‐2BP with A‐D‐π‐D‐A configuration shows a prominent sensitivity of 787 (Ra/Rg) in 20 ppm NH3 at room temperature and an almost initial and stable response under different relative humidity conditions, which is the highest among currently reported OSM sensors. Supported by theoretical calculations and in situ FTIR spectra, it is revealed that B←N units, which function as the active centers mediate the specific ammonia adsorption. This study provides a new understanding of the design of high‐performance room temperature gas sensing materials by decorating B←N units.

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Electron‐Deficient Organic Molecules Based on B←N Unit: A N‐Type Room‐Temperature Chemiresistive Sensors with Moisture Resistance

Wang,

Xing,

Zhang

et al. 2024

Advanced Science

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Organogel Polymer Electrocatalysts for Two‐Electron Oxygen Reduction

Li,

Wang,

Chen

et al. 2024

Small

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Polymer gels, renowned for unparalleled chemical stability and self‐sustaining properties, have garnered significant attention in electrocatalysis. Notably, organic polymer gels that exhibit temperature sensitivity and incorporate suitable polar nonvolatile liquids, enhance electronic conductivity, and impart distinct morphological features, but remain largely unexplored as electrocatalysts for oxygen reduction reaction (ORR). To address this issue, an innovative strategy is proposed for synergistic modulation of the rigidity of mainchain molecular skeleton and length of alkyl sidechains, enabling the development of organogel polymers with a sol–gel temperature‐sensitive phase transition that promises high selectivity and enhanced activity in electrocatalytic processes. Notably, the shortening of alkyl sidechain length can significantly affect the gelation behavior and internal microstructure of the catalyst, which modifies the electron state, ultimately impacting the catalytic activity of the gel polymer catalysts. In particular, phenyl‐containing Ph‐FL1 with short alkyl sidechains demonstrates outstanding 2e− ORR activity in alkaline medium, achieving a remarkable hydrogen peroxide (H2O2) selectivity of 98.6% with an impressive yield of 4.08 mol g−1 h−1. This performance surpasses most metal‐free carbon‐based electrocatalysts. Through theoretical calculation, the carbon atom (site‐3) of C═N group is identified as potential active sites, representing a significant advancement toward designing cost‐effective and efficient ORR electrocatalysts.

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Modulating Oxygen Reduction Activity in Chalcogenophene‐Incorporated Organic Electrocatalysts through Main‐Group Element Engineering

Cheng,

Wang,

Chen

et al. 2024

Small

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Organic small molecules (OSMs) with well‐defined structures are crucial integral components of cathode catalysts for fuel cells. Despite the acknowledged potential of heteroatom doping to enhance the catalytic performance of metal‐free carbon‐based catalysts, there exists a notable gap in conducting molecular structure and catalytic activity, particularly under the premise of maintaining a constant molecular skeleton and with a clear molecular structure. Herein, the charge distribution is modulated by introducing different chalcogens into the same molecular skeleton through main‐group engineering. Among these OSMs, the Se‐containing small molecule OSM‐Se combined with carbonized calcium alginate exhibits a notable quasi‐four‐electron‐transfer oxygen reduction reaction pathway, displaying a superior half‐wave potential (E1/2) of 0.73 V, accompanied by outstanding electrochemical stability. Density functional theory calculations demonstrate that Se‐containing small molecules can enhance the capabilities of catalysts in adsorbing and dissociating oxygen molecules, and contribute to reducing the reaction barrier of the oxygen reduction reaction. This study presents a straightforward yet highly effective approach for metal‐free carbon‐based OSM electrocatalysts.

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Host-guest-induced electronic state triggers two-electron oxygen reduction electrocatalysis

Cited by 5 publications

References 65 publications

Electron‐Deficient Organic Molecules Based on B←N Unit: A N‐Type Room‐Temperature Chemiresistive Sensors with Moisture Resistance

Electron‐Deficient Organic Molecules Based on B←N Unit: A N‐Type Room‐Temperature Chemiresistive Sensors with Moisture Resistance

Organogel Polymer Electrocatalysts for Two‐Electron Oxygen Reduction

Modulating Oxygen Reduction Activity in Chalcogenophene‐Incorporated Organic Electrocatalysts through Main‐Group Element Engineering

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