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Three-in-one oxygen vacancy: whole visible-spectrum absorption, efficient charge separation and surface site activation for robust CO2 photoreduction
摘要： Exploitation of efficient catalysts to realize solar-driven conversion of inert CO2 into useful fuels confronts big challenges owing to the poor photoabsorption, sluggish charge separation and inefficient surface reactive sites of photocatalysts. Herein, we report a facile and controllable in situ reduction strategy to create surface oxygen vacancies (OVs) on Aurivillius-phase Sr2Bi2Nb2TiO12 nanosheets. Sr2Bi2Nb2TiO12 nanosheets are for the first time prepared by a mineralizer-assisted soft-chemical method, and the introduction of OVs on the surface of Sr2Bi2Nb2TiO12 not only extends photo-response region, but also tremendously promotes separation of photo-induced charge carriers. Moreover, the adsorption and activation of CO2 molecules on the surface of the catalyst are largely enhanced. In the gas-solid reaction system without any co-catalysts or sacrificial agents, OVs-abundant Sr2Bi2Nb2TiO12 nanosheets show an outstanding CO2 photoreduction activity in producing CO with a rate of 17.11 μmol g?1 h?1, ~58 times higher than that of the bulk counterpart, surpassing most previously reported state-of-the-art photocatalysts. Our study provides a three-in-one integrated solution to advance the comprehensive performance of photocatalysts for solar-energy conversion and generation of renewable energy.
关键词： Sr2Bi2Nb2TiO12 nanosheets,charge separation,photocatalytic CO2 reduction,oxygen vacancies
更新于2025-09-23 15:23:52
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Monometallic Catalytic Models Hosted in Stable Metal-Organic Frameworks for Tunable CO2 Photoreduction
摘要： The photocatalytic reduction of CO2 to energy carriers has emerged as one of the most promising strategy to alleviate the energy crisis and CO2 pollution, for which the development of catalyst was considered as the determining factor for the accomplishment of this conversion process. In this study, three stably and isostructural metal organic frameworks (denoted as MOF-Ni, MOF-Co and MOF-Cu), have been synthesized and used as heterogeneous catalysts applied into photocatalytic CO2 reduction reaction (CO2RR). It is worth noting that the MOF-Ni exhibited a very high selectivity of 97.7% for photoreducing CO2 to CO, which has exceeded most of the reported MOF-based catalysts in the field. Significantly, the MOFs associated with monometallic catalytic centre offer a simply and precisely structural model which allows us to understand the specific effects of different metal ion species on photoreduction of CO2 as well as reactive mechanism more intuitively.
关键词： Isostructural,Metal-Organic Frameworks,Photocatalytic CO2 Reduction,High Selectivity,Monometallic Catalytic Model,Reactive Mechanism
更新于2025-09-23 15:22:29
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Three-in-one oxygen vacancy: whole visible-spectrum absorption, efficient charge separation and surface site activation for robust CO2 photoreduction
摘要： Exploitation of efficient catalysts to realize solar-driven conversion of inert CO2 into useful fuels confronts big challenges owing to the poor photoabsorption, sluggish charge separation and inefficient surface reactive sites of photocatalysts. Herein, we report a facile and controllable in situ reduction strategy to create surface oxygen vacancies (OVs) on Aurivillius-phase Sr2Bi2Nb2TiO12 nanosheets. Sr2Bi2Nb2TiO12 nanosheets are for the first time prepared by a mineralizer-assisted soft-chemical method, and the introduction of OVs on the surface of Sr2Bi2Nb2TiO12 not only extends photo-response region, but also tremendously promotes separation of photo-induced charge carriers. Moreover, the adsorption and activation of CO2 molecules on the surface of the catalyst are largely enhanced. In the gas-solid reaction system without any co-catalysts or sacrificial agents, OVs-abundant Sr2Bi2Nb2TiO12 nanosheets show an outstanding CO2 photoreduction activity in producing CO with a rate of 17.11 μmol g?1 h?1, ~58 times higher than that of the bulk counterpart, surpassing most previously reported state-of-the-art photocatalysts. Our study provides a three-in-one integrated solution to advance the comprehensive performance of photocatalysts for solar-energy conversion and generation of renewable energy.
关键词： Sr2Bi2Nb2TiO12 nanosheets,oxygen vacancies,charge separation,photocatalytic CO2 reduction
更新于2025-09-23 15:22:29
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Highly Selective Photoreduction of CO <sub/>2</sub> with Suppressing H <sub/>2</sub> Evolution by Plasmonic Au/CdSea??Cu <sub/>2</sub> O Hierarchical Nanostructures under Visible Light
摘要： Here, the photocatalytic CO2 reduction reaction (CO2RR) with the selectivity of carbon products up to 100% is realized by completely suppressing the H2 evolution reaction under visible light (λ > 420 nm) irradiation. To target this, plasmonic Au/CdSe dumbbell nanorods enhance light harvesting and produce a plasmon-enhanced charge-rich environment; peripheral Cu2O provides rich active sites for CO2 reduction and suppresses the hydrogen generation to improve the selectivity of carbon products. The middle CdSe serves as a bridge to transfer the photocharges. Based on synthesizing these Au/CdSe–Cu2O hierarchical nanostructures (HNSs), efficient photoinduced electron/hole (e?/h+) separation and 100% of CO selectivity can be realized. Also, the 2e?/2H+ products of CO can be further enhanced and hydrogenated to effectively complete 8e?/8H+ reduction of CO2 to methane (CH4), where a sufficient CO concentration and the proton provided by H2O reduction are indispensable. Under the optimum condition, the Au/CdSe–Cu2O HNSs display high photocatalytic activity and stability, where the stable gas generation rates are 254 and 123 μmol g?1 h?1 for CO and CH4 over a 60 h period.
关键词： photocatalytic CO2 reduction,plasmonic heterostructures,visible light,H2 evolution
更新于2025-09-23 15:21:01
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Plasmonic Ag@TiO <sub/>2</sub> Core-Shell Nanoparticles for Enhanced CO <sub/>2</sub> Photoconversion to CH <sub/>4</sub>
摘要： Ag@TiO2 nanoparticles (NPs) with Ag metal cores and TiO2 semiconductor shells were prepared with a hydrothermal method and their structure was characterized by scanning electron microscopy, transmission electron microscopy and X-ray diffraction. The core-shell Ag-TiO2 NPs were deposited on a glass plate and employed as photocatalysts for CO2 conversion by irradiation of solar simulator (AM1.5) under CO2 atmosphere. Selective CH4 evolution by CO2 photoconversion was attained with the core-shell Ag@TiO2 NP photocatalyst. The CH4 evolution rate normalized by specific surface areas was ten times higher than those of reference TiO2 NPs and conventional TiO2 NPs with accompanying Ag deposits. The role of the Ag core was also demonstrated in photodecomposition of a dye by the core-shell Ag@TiO2 NPs. These results suggested the high photocatalytic activity of the core-shell Ag@TiO2 NPs was archived due to bandgap improvement of the TiO2 shell and increase of photon flux to the TiO2 shell by the plasmonic Ag core.
关键词： Photocatalytic CO2 Reduction,Surface Plasmonic Resonance,Ag@TiO2,Core-shell Structure,Light Scattering Effect
更新于2025-09-19 17:13:59
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Fabrication of CdS hierarchical multi-cavity hollow particles for efficient visible light CO <sub/>2</sub> reduction
摘要： Designing advanced structures for semiconductor photocatalysts is an effective approach to enhance their performance. However, it is not easy to fabricate functional photocatalytic materials with complex nano-architectures. Here we have developed a sequential solution growth, sulfidation and cation-exchange strategy to fabricate CdS hierarchical multi-cavity hollow particles (HMCHPs). This strategy starts with the growth of Zn-based zeolitic imidazolate framework (ZIF-8) onto cobalt glycerate (Co-G) solid spheres. Sulfidation of the obtained Co-G@ZIF-8 composite particles leads to the formation of CoSx@ZnS HMCHPs, which are converted into CdS HMCHPs via a cation-exchange reaction. Owing to the favourable properties of the well-defined hierarchical hollow structure, the CdS HMCHPs exhibit enhanced activity for photocatalytic CO2 reduction compared with other CdS photocatalysts with solid and common hollow structures. The performance of CdS HMCHPs can be further promoted by loading of Au to reach a CO generation rate of 3758 μmol h?1 g?1 under visible light irradiation.
关键词： Au loading,hierarchical multi-cavity hollow particles,CdS,photocatalytic CO2 reduction,visible light
更新于2025-09-10 09:29:36
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Photoreduction of Carbon Dioxide to Methanol over Copper Based Zeolitic Imidazolate Framework-8: A New Generation Photocatalyst
摘要： The efficient reduction of CO2 into valuable products such as methanol, over metal-organic frameworks (MOFs) based catalyst, has received much attention. The photocatalytic reduction is considered the most economical method due to the utilization of solar energy. In this study, Copper (II)/Zeolitic Imidazolate Framework-8 (Cu/ZIF-8) catalysts were synthesized via a hydrothermal method for photocatalytic reduction of CO2 to methanol. The synthesized catalysts were characterized by X-ray Photoelectron Spectroscopy (XPS), Field Emission Scanning Electron Microscopy (FESEM) coupled with Energy Dispersive X-ray (EDX), Ultraviolet-visible (UV-vis) spectroscopy, and X-Ray Diffraction (XRD). The host ZIF-8, treated with 2 mmol copper prepared in 2M ammonium hydroxide solution showed the highest photocatalytic activity. The crystal structures of ZIF-8 and 2Cu/ZIF-8N2 catalysts were observed as cubic and orthorhombic, respectively and the XPS analysis confirmed the deposition of Cu (II) ions over ZIF-8 surface among all the prepared catalysts. The orthorhombic structure, nano-sized crystals, morphology and Cu loading of the 2Cu/ZIF-8N2 catalyst were the core factors to influence the photocatalytic activity. The yield of Methanol was found to be 35.82 μmol/L·g after 6 h of irradiations on 2Cu/ZIF-8N2 catalyst in the wavelength range between 530–580 nm. The copper-based ZIF-8 catalyst has proven as an alternative approach for the economical photocatalytic reduction of CO2 to CH3OH.
关键词： Cu/ZIF-8,photocatalytic CO2 reduction,methanol production,metal-organic frameworks (MOFs)
更新于2025-09-10 09:29:36
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Development of Graphene Based Photocatalysts for CO2 Reduction to C1 Chemicals: A brief Overview
摘要： Transformation of CO2, a notorious greenhouse gas, to solar fuels is a promising strategy to alleviate the issues of global warming, environmental pollution, and climatic changes. Additionally, the CO2 conversion to useful chemicals/ fuels also possess a great potential to well match the energy demand in a sustainable manner. Hence, such exceptional benefits of harnessing CO2, by capitalizing sunlight, to valuable chemicals/fuels through photocatalysis, as one of the effective approach in the respective domain, have triggered great interest among researchers and scientific community. In this regard, utilization of customary and standard photocatalytic materials, specifically metal oxides like TiO2, are modified to provide enhanced performance, which is usually restricted due to limited intrinsic optical and physicochemical properties. To overcome such a critical issue of limited performance, several strategies like metals and non-metals doping, hetero-junctions, composites and nanostructures formation of photocatalytic materials have been investigated. Recently, with the invention of graphene and its derivatives, graphene based photocatalytic materials have been a topic of great interest, specifically for photocatalysts development and photocatalysis application. Graphene and its derivatives, due to their extraordinary physiochemical and electrical properties like high surface area, stability, anticorrosion capacity, photosensitizer, and excellent conductivity, can knock out the performance limiting constraints faced by traditional photocatalysts. Thus, Graphene based photocatalysts can be a feasible strategy to break new grounds in the field of photocatalytic CO2 reduction (PCCR) to useful chemicals/ fuels, i.e. conversion of sunlight to fuels. Herein, a summarized overview is presented for the latest development in graphene-based photocatalysts, focusing various strategies and researches being investigated in relation to the, utility of graphene and its derivatives for solar fuels generation, particularly C1 chemicals like CO, CH4, CH3OH, and insights to their role in improving efficacy of photocatalysts.
关键词： Photocatalytic activity,Photocatalytic CO2 reduction,Solar fuels,Product Selectivity,Graphene based photocatalysts
更新于2025-09-09 09:28:46
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Highly Efficient and Robust Photocatalytic Systems for CO <sub/>2</sub> Reduction Consisting of a Cu(I) Photosensitizer and Mn(I) Catalysts
摘要： The development of highly efficient, selective, and durable photocatalytic CO2 reduction systems that only use earth-abundant elements is key for both solving global warming and tackling the shortage of energy and carbon resources. Here, we successfully developed CO2 reduction photocatalysts using [Cu2(P2bph)2]2+ (CuPS) (P2bph = 4,7-diphenyl-2,9-di(diphenylphosphinotetramethylene)-1,10-phenanthroline) as a redox photosensitizer and fac-Mn(X2bpy)(CO)3Br (Mn(4X)) (X2bpy = 4,4′-X2-2,2′-bipyridine (X = ?H and ?OMe) or Mn(6mes) (6mes = 6,6′-(mesityl)2-2,2′-bipyridne)) as the catalyst. The most efficient photocatalysis was achieved by Mn(4OMe): The total quantum yield of CO2 reduction products was 57%, the turnover number based on the Mn catalyst was over 1300, and the selectivity of CO2 reduction was 95%. Electronic and steric effects of the substituents (X) in the Mn complexes largely affected both the photocatalytic efficiency and the product selectivity. For example, the highest selectivity of CO formation was achieved by using Mn(6mes) (selectivity SCO = 96.6%), whereas the photocatalytic system using Mn(4H) yielded HCOOH as the main product (SHCOOH = 74.6%) with CO and H2 as minor products (SCO = 23.7%, SH2 = 1.7%). In these photocatalytic reactions, CuPS played its role as an efficient and very durable redox photosensitizer, while remaining stable in the reaction solution even after a turnover number of 200 had been reached (the catalyst used had a turnover number of over 1000).
关键词： turnover number,Cu(I) photosensitizer,Mn(I) catalysts,photocatalytic CO2 reduction,earth-abundant elements,quantum yield,product selectivity
更新于2025-09-09 09:28:46