Three types of photocatalytic systems for CO2 reduction, which were recently developed in our group, are reviewed. First, two-component systems containing different rhenium(I) complexes having different roles; i.e., redox photosensitizer and catalyst in the reaction solution are described. The mixed system of a ring-shaped rhenium(I) trinuclear complex and fac-[Re(bpy)(CO)3(MeCN)](+) is currently the most efficient photocatalytic system for CO2 reduction (ΦCO = 0.82 at λex = 436 nm). The second is a series of supramolecular photocatalysts, which have units with different functions in one molecule, i.e., redox photosensitizer, catalyst, and bridging ligand. The highest durability and speed of photocatalysis were achieved by using this system (ΦCO = 0.45, TONCO = 3029, and TOFCO = 35.7 min(-1)). The third is a novel type of artificial Z-Scheme photocatalyst for CO2 reduction, of which photocatalysis is revealed by stepwise excitation of both a semiconductor photocatalyst unit and the supramolecular photocatalyst unit. This system has both strong oxidation and reduction powers.
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http://dx.doi.org/10.1021/ic502675a | DOI Listing |
J Hazard Mater
January 2025
MOE Key Laboratory of Bio-Intelligent Manufacturing, School of Bioengineering, Dalian University of Technology, Dalian 116024, PR China.
Microalgae-based wastewater treatment could realize simultaneous nutrients recovery and CO sequestration. However, impacts of environmental microplastics (MPs) and antibiotic co-exposure on microalgal growth, nutrients removal, intracellular nitric oxide (NO) accumulation and subsequent nitrous oxide (NO) emission are unclarified, which could greatly offset the CO sequestration benefit. To reveal the potential impacts of environmental concentrations of MPs and antibiotic co-exposure on microalgal greenhouse gas mitigation, this study investigated the effects of representative MPs (PE, PVC, PA), antibiotic sulfamethoxazole (SMX), and nitrite (NO-N) in various combinations on attached Chlorella sorokiniana growth, nutrients removal, anti-oxidative responses, and NO emission originated from intracellular NO build-up.
View Article and Find Full Text PDFAdv Mater
January 2025
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012, China.
The design and synthesis of metal-organic frameworks (MOFs) with outstanding light-harvesting and photoexcitation for artificial photocatalytic CO reduction is an attractive but challenging task. In this work, a novel aggregation-induced emission (AIE)-active ligand, tetraphenylpyrazine (PTTBPC) is proposed and utilized for the first time to construct a Zr-MOF photocatalyst via coordination with stable Zr-oxo clusters. Zr-MOF is featured by a scu topology with a two-fold interpenetrated framework, wherein the PTTBPC ligands enable strong light-harvesting and photoexcitation, while the Zr-oxo clusters facilitate CO adsorption and activation, as well as offer potential sites for further metal modification.
View Article and Find Full Text PDFSmall
January 2025
National Energy Metal Resources and New Materials Key Laboratory, Engineering Research Center of the Ministry of Education for Advanced Battery Materials, Hunan Provincial Key Laboratory of Nonferrous Value-Added Metallurgy, School of Metallurgy and Environment, Central South University, Changsha, 410083, P. R. China.
Electrochemical CO reduction (CORR) in membrane electrode assembly (MEA) represents a viable strategy for converting CO into value-added multi-carbon (C) compounds. Therefore, the microstructure of the catalyst layer (CL) affects local gas transport, charge conduction, and proton supply at three-phase interfaces, which is significantly determined by the solvent environment. However, the microenvironment of the CLs and the mechanism of the solvent effect on C selectivity remains elusive.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Hefei National Research Center for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China.
The local electric field (LEF) plays an important role in the catalytic process; however, the precise construction and manipulation of the electric field microenvironment around the active site remains a significant challenge. Here, we have developed a supramolecular strategy for the implementation of a LEF by introducing the host macrocycle 18-crown-6 (18C6) into a cobalt phthalocyanine (CoPc)-containing covalent organic framework (COF). Utilizing the supramolecular interaction between 18C6 and potassium ion (K), a locally enhanced K concentration around CoPc can be built to generate a LEF microenvironment around the catalytically active Co site.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
Shanxi Coal International Energy Group Co., Ltd., Taiyuan 030000, China.
Photocatalytic reduction of CO will play a major role in future energy and environmental crisis. To investigate the adsorption mechanisms of CO and HO molecules involved in the catalytic process on the surface of anatase titanium dioxide 101 (TiO(101)) and the influence of Au atom doping on their adsorption, first-principles density functional theory calculations were used. The results show that 1.
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