材料科学
电合成
多孔性
化学工程
金属
纳米技术
封装(网络)
无机化学
电化学
冶金
物理化学
复合材料
电极
计算机网络
化学
计算机科学
工程类
作者
Yilei He,Yanze Wei,Zumin Wang,Tian Xia,Rao Fu,Zhifan Song,Ranbo Yu
标识
DOI:10.1002/adfm.202314654
摘要
Abstract Tuning the electrocatalytic selectivity and long‐term stability for industrially significant, yet reactively unfavorable products, remains a challenge in oxygen reduction. Herein, the Au/TiO 2 catalysts with strong metal–support interactions (SMSI) are designed and synthesized through an in situ auto‐reduction of Au‐modified Ti‐MOF. Highly dispersed ultra‐low loading of Au NPs strongly capsulated in porous TiO 2 substrate, together with conductive carbon derivated from MOFs, enables Au/TiO 2 electrocatalysts to achieve excellent H 2 O 2 electrosynthesis through the two‐electron oxygen reduction reaction (2e ORR). Au(1.0)/TiO 2 (0.52 wt% Au loading) exhibited a high selectivity of 90%, a remarkable Faradaic efficiency of 98%, and 72.2 mg L −1 h −1 H 2 O 2 production. Highly dispersed Au NPs promote active site exposure, while the conductive carbon and the porous superstructure enhance mass diffusion. Notably, the SMSI between Au NPs and TiO 2 substrate leads to superb stability (over 168 h) of the electrocatalysts, as it ensures continuous electronic interactions. Experimental characterizations and density functional theory (DFT) simulations further revealed that the SMSI effect medicates the activation of the *OOH intermediate formation and the d‐band center, which are conductive to 2e ORR. Moreover, this strategy provides a potential way toward high‐performance electrocatalysts in flow system devices for continuously purifying sewage and chemical bleaching in extreme environments.
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