磷烯光催化分解水研究进展

半导体光催化分解水被认为是解决全球能源短缺和环境污染问题的潜在途径之一。近年来, 磷烯(BP)由于具有带隙可调、空穴迁移率高、吸收光谱宽等特性而在光催化分解水方面得到了广泛关注。本文综述了国内外近年来在磷烯光催化分解水领域所取得的重要研究进展, 总结了磷烯基光催化剂的合成方法、表面修饰和异质结构构建等改性策略, 阐述了磷烯基光催化剂的构-效关系和电荷转移机制, 并展望了磷烯基光催化剂所面临的机遇和挑战, 揭示了磷烯基材料在太阳能利用和转化方面的重要应用潜力。     

Design of Heterostructured Hollow Photocatalysts for Solar‐to‐Chemical Energy Conversion

Direct conversion of solar energy into chemical energy in a sustainable manner is one of the most promising solutions to the energy crisis and environmental issues. Fabrication of highly active photocatalysts is of great significance for the practical applications of efficient solar‐to‐chemical energy conversion systems. Among various photocatalytic materials, semiconductor‐based heterostructured photocatalysts with hollow features show distinct advantages. Recent research efforts on rational design of heterostructured hollow photocatalysts toward photocatalytic water splitting and CO₂ reduction are presented. First, both single‐shelled and multishelled heterostructured photocatalysts are surveyed. Then, heterostructured hollow photocatalysts with tube‐like and frame‐like morphologies are discussed. It is intended that further innovative works on the material design of high‐performance photocatalysts for solar energy utilization can be inspired.     

Recent Progress of Single-Atom Photocatalysts Applied in Energy Conversion and Environmental Protection

Photocatalysis driven by solar energy is a feasible strategy to alleviate energy crises and environmental problems. In recent years, significant progress has been made in developing advanced photocatalysts for efficient solar-to-chemical energy conversion. Single-atom catalysts have the advantages of highly dispersed active sites, maximum atomic utilization, unique coordination environment, and electronic structure, which have become a research hotspot in heterogeneous photocatalysis. This paper introduces the potential supports, preparation, and characterization methods of single-atom photocatalysts in detail. Subsequently, the fascinating effects of single-atom photocatalysts on three critical steps of photocatalysis (the absorption of incident light to produce electron-hole pairs, carrier separation and migration, and interface reactions) are analyzed. At the same time, the applications of single-atom photocatalysts in energy conversion and environmental protection (CO₂ reduction, water splitting, N₂ fixation, organic macromolecule reforming, air pollutant removal, and water pollutant degradation) are systematically summarized. Finally, the opportunities and challenges of single-atom catalysts in heterogeneous photocatalysis are discussed. It is hoped that this work can provide insights into the design, synthesis, and application of single-atom photocatalysts and promote the development of high-performance photocatalytic systems.     

Modulation of Bi2MoO6‐Based Materials for Photocatalytic Water Splitting and Environmental Application: a Critical Review

Highly active photocatalysts driving chemical reactions are of paramount importance toward renewable energy substitutes and environmental protection. As a fascinating Aurivillius phase material, Bi₂MoO₆ has been the hotspot in photocatalytic applications due to its visible light absorption, nontoxicity, low cost, and high chemical durability. However, pure Bi₂MoO₆ suffers from low efficiency in separating photogenerated carriers, small surface area, and poor quantum yield, resulting in low photocatalytic activity. Various strategies, such as morphology control, doping/defect‐introduction, metal deposition, semiconductor combination, and surface modification with conjugative π structures, have been systematically explored to improve the photocatalytic activity of Bi₂MoO₆. To accelerate further developments of Bi₂MoO₆ in the field of photocatalysis, this comprehensive Review endeavors to summarize recent research progress for the construction of highly efficient Bi₂MoO₆‐based photocatalysts. Furthermore, benefiting from the enhanced photocatalytic activity of Bi₂MoO₆‐based materials, various photocatalytic applications including water splitting, pollutant removal, and disinfection of bacteria, were introduced and critically reviewed. Finally, the current challenges and prospects of Bi₂MoO₆ are pointed out. This comprehensive Review is expected to consolidate the existing fundamental theories of photocatalysis and pave a novel avenue to rationally design highly efficient Bi₂MoO₆‐based photocatalysts for environmental pollution control and green energy development.     

Graphene in Photocatalysis: A Review

In recent years, heterogeneous photocatalysis has received much research interest because of its powerful potential applications in tackling many important energy and environmental challenges at a global level in an economically sustainable manner. Due to their unique optical, electrical, and physicochemical properties, various 2D graphene nanosheets‐supported semiconductor composite photocatalysts have been widely constructed and applied in different photocatalytic fields. In this review, fundamental mechanisms of heterogeneous photocatalysis, including thermodynamic and kinetics requirements, are first systematically summarized. Then, the photocatalysis‐related properties of graphene and its derivatives, and design rules and synthesis methods of graphene‐based composites are highlighted. Importantly, different design strategies, including doping and sensitization of semiconductors by graphene, improving electrical conductivity of graphene, increasing eloectrocatalytic active sites on graphene, strengthening interface coupling between semiconductors and graphene, fabricating micro/nano architectures, constructing multi‐junction nanocomposites, enhancing photostability of semiconductors, and utilizing the synergistic effect of various modification strategies, are thoroughly summarized. The important applications including photocatalytic pollutant degradation, H₂ production, and CO₂ reduction are also addressed. Through reviewing the significant advances on this topic, it may provide new opportunities for designing highly efficient 2D graphene‐based photocatalysts for various applications in photocatalysis and other fields, such as solar cells, thermal catalysis, separation, and purification.     

Ultrathin 2D Photocatalysts: Electronic‐Structure Tailoring,Hybridization, and Applications

As a sustainable technology, semiconductor photocatalysis has attracted considerable interest in the past several decades owing to the potential to relieve or resolve energy and environmental‐pollution issues. By virtue of their unique structural and electronic properties, emerging ultrathin 2D materials with appropriate band structure show enormous potential to achieve efficient photocatalytic performance. Here, the state‐of‐the‐art progress on ultrathin 2D photocatalysts is reviewed and a critical appraisal of the classification, controllable synthesis, and formation mechanism of ultrathin 2D photocatalysts is presented. Then, different strategies to tailor the electronic structure of ultrathin 2D photocatalysts are summarized, including component tuning, thickness tuning, doping, and defect engineering. Hybridization with the introduction of a foreign component and maintaining the ultrathin 2D structure is presented to further boost the photocatalytic performance, such as quantum dots/2D materials, single atoms/2D materials, molecular/2D materials, and 2D–2D stacking materials. More importantly, the advancement of versatile photocatalytic applications of ultrathin 2D photocatalysts in the fields of water oxidation, hydrogen evolution, CO₂ reduction, nitrogen fixation, organic syntheses, and removal pollutants is discussed. Finally, the future opportunities and challenges regarding ultrathin 2D photocatalysts to bring about new opportunities for future research in the field of photocatalysis are also presented.     

Smart Utilization of Carbon Dots in Semiconductor Photocatalysis

Efficient capture of solar energy will be critical to meeting the energy needs of the future. Semiconductor photocatalysis is expected to make an important contribution in this regard, delivering both energy carriers (especially H₂) and valuable chemical feedstocks under direct sunlight. Over the past few years, carbon dots (CDs) have emerged as a promising new class of metal‐free photocatalyst, displaying semiconductor‐like photoelectric properties and showing excellent performance in a wide variety of photoelectrochemical and photocatalytic applications owing to their ease of synthesis, unique structure, adjustable composition, ease of surface functionalization, outstanding electron‐transfer efficiency and tunable light‐harvesting range (from deep UV to the near‐infrared). Here, recent advances in the rational design of CDs‐based photocatalysts are highlighted and their applications in photocatalytic environmental remediation, water splitting into hydrogen, CO₂ reduction, and organic synthesis are discussed.     

Tantalum (Oxy)Nitride: Narrow Bandgap Photocatalysts for Solar Hydrogen Generation

Photocatalytic water splitting, which directly converts solar energy into hydrogen, is one of the most desirable solar-energy-conversion approaches. The ultimate target of photocatalysis is to explore efficient and stable photocatalysts for solar water splitting. Tantalum (oxy)nitride-based materials are a class of the most promising photocatalysts for solar water splitting because of their narrow bandgaps and sufficient band energy potentials for water splitting. Tantalum (oxy)nitride-based photocatalysts have experienced intensive exploration, and encouraging progress has been achieved over the past years. However, the solar-to-hydrogen (STH) conversion efficiency is still very far from its theoretical value. The question of how to better design these materials in order to further improve their water-splitting capability is of interest and importance. This review summarizes the development of tantalum (oxy)nitride-based photocatalysts for solar water spitting. Special interest is paid to important strategies for improving photocatalytic water-splitting efficiency. This paper also proposes future trends to explore in the research area of tantalum-based narrow bandgap photocatalysts for solar water splitting.     

二硫化钼纳米材料在光催化应用中的研究进展

二硫化钼(MoS_2)具有类石墨烯层状结构、良好的光学性能和电子传输特性,在光催化、太阳能电池、光开关等领域具有广阔的应用前景,一直备受关注。综述了近5年MoS_2纳米材料在光催化降解有机物和光催化水解制氢领域内的最新研究进展,分析了MoS_2纳米材料在光催化应用中存在的主要问题与挑战,重点介绍了相关解决方法。最后展望了MoS_2纳米材料在光催化应用中的发展方向和应用前景。     

Plasmonic-metal nanostructures for efficient conversion of solar to chemical energy

Recent years have seen a renewed interest in the harvesting and conversion of solar energy. Among various technologies, the direct conversion of solar to chemical energy using photocatalysts has received significant attention. Although heterogeneous photocatalysts are almost exclusively semiconductors, it has been demonstrated recently that plasmonic nanostructures of noble metals (mainly silver and gold) also show significant promise. Here we review recent progress in using plasmonic metallic nanostructures in the field of photocatalysis. We focus on plasmon-enhanced water splitting on composite photocatalysts containing semiconductor and plasmonic-metal building blocks, and recently reported plasmon-mediated photocatalytic reactions on plasmonic nanostructures of noble metals. We also discuss the areas where major advancements are needed to move the field of plasmon-mediated photocatalysis forward.     

Defect‐Tailoring Mediated Electron–Hole Separation in Single‐Unit‐Cell Bi3O4Br Nanosheets for Boosting Photocatalytic Hydrogen Evolution and Nitrogen Fixation

Solar photocatalysis is a potential solution to satisfying energy demand and its resulting environmental impact. However, the low electron–hole separation efficiency in semiconductors has slowed the development of this technology. The effect of defects on electron–hole separation is not always clear. A model atomically thin structure of single‐unit‐cell Bi₃O₄Br nanosheets with surface defects is proposed to boost photocatalytic efficiency by simultaneously promoting bulk‐ and surface‐charge separation. Defect‐rich single‐unit‐cell Bi₃O₄Br displays 4.9 and 30.9 times enhanced photocatalytic hydrogen evolution and nitrogen fixation activity, respectively, than bulk Bi₃O₄Br. After the preparation of single‐unit‐cell structure, the bismuth defects are controlled to tune the oxygen defects. Benefiting from the unique single‐unit‐cell architecture and defects, the local atomic arrangement and electronic structure are tuned so as to greatly increase the charge separation efficiency and subsequently boost photocatalytic activity. This strategy provides an accessible pathway for next‐generation photocatalysts.     

Enhancement of Solar‐Driven Photocatalytic Activity of BiOI Nanosheets through Predominant Exposed High Energy Facets and Vacancy Engineering

The increasing application of exposed high energy facet is an effective strategy to improve the photocatalytic performance of photocatalysts because the vacancies are beneficial to photocatalytic reaction. Vacancy dominates numerous distinct properties of semiconductor materials and thus plays a conclusive role in the photocatalysis applications. In this work, two kinds of BiOI nanomaterials with different vacancies are synthesized via a facile solvothermal method. The positron annihilation analysis shows that the thinner BiOI nanosheets possess larger‐sized vacancy than BiOI nanoplates. Thus, BiOI nanosheets show the enhanced separation efficiency of electron–hole pairs and adsorption ability for contaminants under visible light. The results are also validated with the first‐principle computation. Therefore, higher photocatalytic activity to the photodegradation of tetracycline is observed from the nanosheets than that obtained from BiOI nanoplates. This work not only arouses attention to vacancies, but also opens up an avenue for precision design of vacancies to prepare novel photocatalytic materials driven under solar light.     

Fabrication and photocatalytic activity of TiO2 nanofiber membrane

Titanium dioxide is one of the best semiconductor photocatalysts available for photocatalysis. In this paper, titanium dioxide nanofiber membranes are prepared by post-anneal-assisted electrospinning process. The obtained membrane is composed of anatase titanium dioxide continuous and porous nanofibers with diameters ranging from 65 to 115 nm. An optimized annealing scheme is determined. Photocatalytic measurements show that the photocatalytic efficiency of the anatase TiO₂ nanofiber membrane is 72%, which is highly superior to that of the anatase TiO₂ thin film (44%). It is believed that the large specific surface area intensively enhances the photocatalytic reactions and the good shape retention might be favorable for recuperability and practicality. The potential applications for environmental purification are discussed.     

Carbon–Graphitic Carbon Nitride Hybrids for Heterogeneous Photocatalysis

Polymeric graphitic carbon nitride (g-C₃N₄) and various carbon materials have experienced a renaissance as viable alternates in photocatalysis due to their captivating metal-free features, favorable photoelectric properties, and economic adaptabilities. Although numerous efforts have focused on the integration of both materials with optimized photocatalytic performance in recent years, the direct parameters for this emerging enhancement are not fully summarized yet. Fully understanding the synergistic effects between g-C₃N₄ and carbon materials on photocatalytic action is vital to further development of metal-free semiconductors in future studies. Here, recent advances of carbon/g-C₃N₄ hybrids on various photocatalytic applications are reviewed. The dominant governing factors by inducing carbon into g-C₃N₄ photocatalysts with involving photocatalytic mechanism are highlighted. Five typical carbon-induced enhancement effects are mainly discussed here, i.e., local electric modification, band structure tailoring, multiple charge carrier activation, chemical group functionalization, and abundant surface-modified engineering. Photocatalytic performance of carbon-induced g-C₃N₄ photocatalysts for addressing directly both the renewable energy storage and environmental remediation is also summarized. Finally, perspectives and ongoing challenges encountered in the development of metal-free carbon-induced g-C₃N₄ photocatalysts are presented.     

Cyclic performance and photo-induced crystalline growth of nanostructured AgI/TiO2 visible light photocatalyst

Nanostructured AgI/TiO2 visible light photocatalyst was prepared with AgNO3, KI, and Ti(OBu)4 as precursors. The photocatalyst was used repeatedly to degrade methylene blue and methyl orange in water with visible light irradiation. Though a high photocatalytic efficiency was observed for the photocatalyst in the first cycle, the photocatalytic efficiency was found to decrease dramatically in subsequent cycles. X-ray diffraction and SEM analyses revealed an obvious crystalline growth of AgI in AgI/TiO2 nanocomposite after photocatalysis or visible light irradiation. It was proposed that photo-induced crystalline growth had occurred to AgI in the course of photocatalysis and resulted in dramatic decrease in the photocatalytic efficiency of the photocatalyst. Photo-induced crystalline growth may be a limiting factor for the lifetime of photocatalysts and should be examined as an important aspect of photostability when new photocatalysts are developed.     

Recent Advances in Conjugated Polymers for Visible-Light-Driven Water Splitting

With the ambition of solving the challenges of the shortage of fossil fuels and their associated environmental pollution, visible-light-driven splitting of water into hydrogen and oxygen using semiconductor photocatalysts has emerged as a promising technology to provide environmentally friendly energy vectors. Among the current library of developed photocatalysts, organic conjugated polymers present unique advantages of sufficient light-absorption efficiency, excellent stability, tunable electronic properties, and economic applicability. As a class of rising photocatalysts, organic conjugated polymers offer high flexibility in tuning the framework of the backbone and porosity to fulfill the requirements for photocatalytic applications. In the past decade, significant progress has been made in visible-light-driven water splitting employing organic conjugated polymers. The recent development of the structural design principles of organic conjugated polymers (including linear, crosslinked, and supramolecular self-assembled polymers) toward efficient photocatalytic hydrogen evolution, oxygen evolution, and overall water splitting is described, thus providing a comprehensive reference for the field. Finally, current challenges and perspectives are also discussed.     

新型复合纳米材料用于光催化降解染料废水的研究进展EI北大核心CSCD

光催化技术是解决当今人类社会中环境问题和能源危机两大问题的有效途径,半导体材料在早期的研究中备受青睐。然而,单一半导体光催化剂存在可见光响应程度差、电子空穴对易复合等缺点,光催化技术在降解染料废水的应用中有效率较低,因此研究者对新型复合纳米材料作为光催化剂降解染料废水进行了深入的研究。本文介绍了石墨烯、金属有机骨架、碳量子点三种新型复合纳米材料用于光催化降解染料废水中污染物的研究进展和主要研究结果,按照复合纳米材料设计升级的思路,简述了部分新型复合纳米材料的制备方法,对目标污染物的降解率进行了分析。通过总结新型光催化材料降解水中污染物的性能,对未来发展趋势进行了展望,指出新型复合纳米材料在光催化方向今后的发展趋势和研究重点是有针对性的处理废水,并实现工业化。     

g-C3N4光催化性能的研究进展

利用光催化剂将太阳能转化为人类可以直接利用的能量, 并用其解决地球资源的枯竭和生存环境的恶化是可再生清洁能源研究的一个方向。g-C₃N₄的独特结构赋予其良好的光催化性能, 使之成为光催化领域的研究热点。目前在光催化领域, g-C₃N₄主要用于催化污染物分解、水解制氢制氧、有机合成及氧气还原。在实际应用中, 为进一步提高g-C₃N₄的光催化效果, 科研工作者开发了多种改进方法, 例如物理复合改性、化学掺杂改性、微观结构调整等。本文主要论述了g-C₃N₄在光催化领域的应用以及光催化性能的改进方法, 简要阐述了光催化和各种改进方法的机理, 分析了目前g-C₃N₄在光催化领域面临的问题和挑战, 展望了g-C₃N₄的应用前景。     

Polymeric Photocatalysts Based on Graphitic Carbon Nitride

Semiconductor‐based photocatalysis is considered to be an attractive way for solving the worldwide energy shortage and environmental pollution issues. Since the pioneering work in 2009 on graphitic carbon nitride (g‐C₃N₄) for visible‐light photocatalytic water splitting, g‐C₃N₄‐based photocatalysis has become a very hot research topic. This review summarizes the recent progress regarding the design and preparation of g‐C₃N₄‐based photocatalysts, including the fabrication and nanostructure design of pristine g‐C₃N₄, bandgap engineering through atomic‐level doping and molecular‐level modification, and the preparation of g‐C₃N₄‐based semiconductor composites. Also, the photo­catalytic applications of g‐C₃N₄‐based photocatalysts in the fields of water splitting, CO₂ reduction, pollutant degradation, organic syntheses, and bacterial disinfection are reviewed, with emphasis on photocatalysis promoted by carbon materials, non‐noble‐metal cocatalysts, and Z‐scheme heterojunctions. Finally, the concluding remarks are presented and some perspectives regarding the future development of g‐C₃N₄‐based photocatalysts are highlighted.     

异相光催化原理、TiO2光催化剂的应用和研究进展

从光吸收过程、表面态光生载流子的俘获和光催化量子效率方面详细地阐述了光催化机理,并概述了TiO2系光催化剂在环境物质净化处理和太阳能转换利用等.最后总结了TiO2系光催化剂的研究现状,如掺杂改性、合成介孔尺度的纳米结构TiO2等.