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A small organic molecule strategy for remedying oxygen vacancies by bismuth defects in BiOBr nanosheet with excellent photocatalytic CO_(2)reduction

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Nano Research 2024年第1期17卷 297-306页

作者： Jing Xie Zhenjiang Lu Yue Feng Jianguo Huang Jindou Hu Aize Hao Yali Cao State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources College of ChemistryXinjiang UniversityUrumqi 830046China

Defect modulation currently plays a decisive role in addressing the poor photoabsorption,sluggish electron hole separation,and high CO_(2)activation barrier in photocatalytic CO_(2)reduction.However,hunting for a straightforward strategy to balance the concentration of oxygen vacancy and metal cation defect in one photocatalyst is still a great challenge.Herein,a bismuth vacancies BiOBr nanosheets(BiOBr-1)on the exposed[001]facets were constructed via an acetic acid molecule modification strategy,which can repair oxygen defect by bismuth vacancy in low-temperature solid-state chemical method.Benefiting from the formed bismuth defects that can not only broaden light absorption and elevate charge separation efficiency,but also enhance adsorption and activation of CO_(2)molecules,the evolution rates of photocatalytic CO_(2)conversion into CO(71.23μmol·g^(-1)·h^(-1))and CH4(8.90μmol·g^(-1)·h^(-1))attained by BiOBr-1 are superior 7.1 and 11 times to that of plate-like BiOBr.The photocatalytic mechanisms including adsorption concentration and activation process of CO_(2)are further revealed by the in situ diffuse reflectance infrared flourier transform spectra(DRIFTS).This finding of the existence of distinct defects in ultrathin nanosheets undoubtedly leads to new possibilities for photocatalyst design using two-dimensional materials with high solar-driven photocatalytic activity.

关键词： solid-state synthesis BiOBr metal vacancies photocatalysis carbon dioxide reduction

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Sub-2 nm IrO_(2)/Ir nanoclusters with compressive strain and metal vacancies boost water oxidation in acid

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Nano Research 2023年第1期16卷 334-342页

作者： Zhijuan Liu Guangjin Wang Jinyu Guo Shuangyin Wang Shuang-Quan Zang Henan Key Laboratory of Crystalline Molecular Functional Materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis Centerand College of ChemistryZhengzhou UniversityZhengzhou 450001China Hunan University State Key Laboratory of Chem/Bio-sensing and ChemometricsCollege of Chemistry and Chemical EngineeringChangsha 410082China School of Materials Science and Energy Engineering Foshan UniversityFoshan 528000China

IrO_(2)exhibits good stability but limited electrocatalytic activity for oxygen evolution reaction in acid.Defect engineering is an effective strategy to improve the intrinsic ability of electrocatalysts by tailoring their electronic structure.Herein,we have successfully synthesized IrO_(2)/Ir heterophase with compressive strain and metal vacancies via a simple substitution-etching method.In virtue of the solubility of Cr in strong alkali,metal vacancies could be formed at surface after etching Cr-doped IrO_(2)/Ir in alkali,which leaded to modulated electronic structure.Meanwhile,the substitution of Cr with smaller atom radius would induce the formation of compressive strain and the relocated atoms made the d-band center shifted.With the regulated electronic structure and tuned d-band center,the obtained electrocatalyst only needed 285 mV to reach 10 mA·cm^(−2)in 0.1 M HClO4.Reaction kinetic has been rapidly accelerated as indicated by the smaller Tafel slope and charge transfer resistance.Theoretical calculations revealed that the d-band center and charge density distribution have been regulated with the introduction of defects in IrO_(2)/Ir,which significantly decreased the free energy barrier of rate determining step.This work provides a valuable reference to design effective and defects-rich electrocatalysts.

关键词： IrO_(2)/Ir nanoclusters compressive strain metal vacancies d-band center water oxidation in acid

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