Solar-driven photocatalytic reactions can mildly activate hydrocarbon C-H bonds to produce value-added chemicals. However, the inefficient utilization of photogenerated carriers hinders the application. Here, we report reversible photochromic BiOBr (denoted as -BiOBr) nanosheets that were colored by trapping photogenerated holes upon visible light irradiation and bleached by water oxidation to generate hydroxyl radicals, demonstrating enhanced carrier separation and water oxidation. The photocatalytic coupling and oxidation reactions of ethylbenzene were efficiently realized by -BiOBr in a water-based medium under ambient temperature and pressure (apparent quantum yield is 14 times that of pristine BiOBr). The -BiOBr nanosheets feature lattice disordered defects on the surface, providing rich uncoordinated catalytic sites and inducing structural distortions and lattice strain, which further leads to an altered band structure and significantly enhanced photocatalytic performances. These hole-trapping materials open up the possibility of substantially elevating the utilization efficiency of photogenerated holes for high-efficiency photocatalytic activation of various saturated C-H bonds.
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http://dx.doi.org/10.1021/jacs.1c10112 | DOI Listing |
J Xenobiot
December 2024
Department of Chemical Engineering, University of Pretoria, Pretoria 0028, South Africa.
The direct discharge of cationic surfactants into environmental matrices has exponentially increased due to their wide application in many products. These compounds and their degraded products disrupt microbial dynamics, hinder plant survival, and affect human health. Therefore, there is an urgent need to develop electroanalytical assessment techniques for their identification, determination, and monitoring.
View Article and Find Full Text PDFInorg Chem
December 2024
Henan Key Laboratory of Polyoxometalate Chemistry, College of Chemistry and Molecular Sciences, Henan University, Kaifeng, Henan 475004, P. R. China.
Amide compounds are widely present in drug molecules and natural products, which can be synthesized by acid-amine condensation. It is urgent to design new photocatalysts for achieving both nitroaromatic reduction and C-H oxidation to obtain raw materials, carboxylic acids, and aromatic amines. Herein, a novel isopolymolybdate-incorporated photoactive metal-organic framework, -TPT, was constructed by combining the oxidation catalyst [MoO], Ni(II) cation, and photosensitive ligand 2,4,6-tri(4-pyridyl)-1,3,5-triazine (TPT).
View Article and Find Full Text PDFACS Appl Mater Interfaces
December 2024
State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, P. R. China.
Proton-electron transfer (PET) processes play a pivotal role in numerous electrochemical reactions; yet, effectively harnessing them remains a formidable challenge. Consequently, unveiling the PET pathway is imperative to elucidate the factors influencing the efficiency and selectivity of small molecule electrochemical conversion. In this study, a Zn-NC model catalyst with N and C vacancies was synthesized using a hydriding method to investigate the universal impact of PET on CO electroreduction.
View Article and Find Full Text PDFJ Am Chem Soc
December 2024
Henan Key Laboratory of Crystalline Molecular Functional Materials, College of Chemistry, Zhengzhou University, Zhengzhou 450001, China.
The conversion of methane and carbon dioxide to form C products is of great interest but presents a long-standing grand challenge due to the significant obstacle of activating the inert C-H and C═O bonds as well as forming the C-C bonds. Herein, the consecutive C-C coupling of CH and CO was realized by using heteronuclear metal cations CuTa, and the desorption of HC═C═O molecules was evidenced by state-of-the-art mass spectrometry. The CuTa reaction system is significantly different from the homonuclear metal systems of Cu and Ta.
View Article and Find Full Text PDFFront Chem
December 2024
Department of Chemistry and Biochemistry, Auburn University, Auburn, AL, United States.
High-level quantum chemical calculations are performed for the (NH)MO and (NH)MO species (M = Ti-Cu), extending our previous work on the bare MO ions. The potential energy curves along the M-O distance are constructed for the ground and multiple excited electronic states of (NH)MO and are compared to those of MO. We see that ammonia stabilizes the oxo states (MO) over the oxyl (MO) ones.
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