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Recent advances in wireless photofixation of dinitrogen to ammonia under the ambient condition: A review 环境条件下二氮无线固氨研究进展综述
IF 13.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2021-06-01 DOI: 10.1016/j.jphotochemrev.2021.100402

Ammonia is the most necessitate and second largely produces chemical reagent worldwide to address the need of the fertilizer industry, as a precursor for many value-added chemicals and a competing source (17.6 wt% H2) for the blooming hydrogen economy. Although N2 constitutes 78.09 % of the earth's atmosphere, however, its conversion to ammonia is strenuous because of its non-polar and triple bond character. To address the burgeoning demand, ammonia is typically synthesized via the conventional energy and capital intensive Haber-Bosch technique utilizing natural gas and releasing tons of (CO2) to the environment. On this basis, cost-effective photon-driven dinitrogen reduction reaction (NRR) is aroused thriving attention as a sustainable and eco-friendly process for ammonia production under ambient conditions. Yet, the photocatalytic ammonia production is not up to the mark for industrial application due to low conversion rate, less catalytic selectivity, ambiguous mechanism, and limited faradic or solar-to-chemical efficiency. Further, the NRR activity of a catalyst essentially depends upon its electronic and surface texture; hence the fabrication of advanced materials is of paramount interest to enhance the performance. The present review covers the underlying mechanism of N2 photoreduction, prevailing theories, different catalytic engineering techniques, various detection methods, and critical challenges encountered in the theme of photofixation of dinitrogen to ammonia. Additionally, the overarching goal of this review is to bestow an outline of recent research articles in earmarking high-caliber photocatalytic systems and hence planting a strong foundation to ensure the succeeding improvement in this promising and hastily stretching field of dinitrogen photofixation research.

氨是世界上最必要的、第二大生产的化学试剂,以满足肥料工业的需求,作为许多增值化学品的前体,也是蓬勃发展的氢经济的竞争来源(17.6 wt% H2)。虽然氮气占地球大气的78.09%,但由于它的非极性和三键特性,它转化为氨是很困难的。为了满足日益增长的需求,氨通常是通过传统的能源和资本密集型的哈伯-博世技术合成的,利用天然气并向环境释放大量二氧化碳。在此基础上,低成本的光子驱动氮还原反应(NRR)作为一种环境条件下可持续、环保的合成氨工艺引起了人们的广泛关注。然而,由于光催化制氨的转化率低、催化选择性差、机理不明确以及faradic或solar-to- chemistry效率有限等问题,目前光催化制氨还没有达到工业应用的标准。此外,催化剂的NRR活性基本上取决于其电子结构和表面结构;因此,先进材料的制造是提高性能的最重要的兴趣。本文综述了氮气光还原的基本机理、主要理论、不同的催化工程技术、各种检测方法以及在二氮固氨这一主题中遇到的关键挑战。此外,本综述的总体目标是概述最近在指定高水平光催化系统方面的研究文章,从而为确保这一前景广阔且迅速发展的二氮光固定研究领域的后续发展奠定坚实的基础。
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引用次数: 15
Light-conversion phosphor nanoarchitectonics for improved light harvesting in sensitized solar cells 光转换荧光粉纳米结构改善敏化太阳能电池的光收集
IF 13.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2021-06-01 DOI: 10.1016/j.jphotochemrev.2021.100404

Photovoltaic technology provides a promising approach for solar energy conversion. One significant factor limiting the efficiency is the poor light harvesting of solar energy, which is related to the mismatch between the energy distribution of photons and the absorption of semiconductor materials or dye. Light-conversion phosphors have been explored as spectral converters to improve the light-harvesting ability in sensitized solar cells. Many progressive studies have been conducted to expand the family of light-conversion phosphors and exploit their application in sensitized solar cells, bringing emerging opportunities to develop commercial sensitized solar cells. In this review, we survey the development of light-conversion phosphors in sensitized solar cells. First, the application and conversion mechanism of light-conversion phosphors, including up-conversion phosphors, down-conversion phosphors, up/down conversion phosphors, and long-lasting phosphors, are summarized in detail. After that, the challenging problems and possible solutions of applying light-conversion phosphors to sensitized solar cells are discussed. The review also highlights some new ideas in the development of sensitized solar cells and the application of light-conversion phosphors in other solar technology.

光伏技术为太阳能转换提供了一种很有前途的途径。限制效率的一个重要因素是太阳能的光收集不良,这与光子的能量分布与半导体材料或染料的吸收之间的不匹配有关。光转换荧光粉作为光谱转换器被用于提高敏化太阳能电池的光收集能力。在扩大光转换荧光粉家族和开发其在敏化太阳能电池中的应用方面进行了许多进展研究,为开发商业化的敏化太阳能电池带来了新的机遇。本文综述了光敏化太阳能电池中光转换荧光粉的研究进展。首先,详细总结了光转换荧光粉的应用和转换机理,包括上转换荧光粉、下转换荧光粉、上/下转换荧光粉和长效荧光粉。然后,讨论了将光转换荧光粉应用于敏化太阳能电池的挑战问题和可能的解决方案。本文还重点介绍了敏化太阳能电池的发展以及光转换荧光粉在其他太阳能技术中的应用。
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引用次数: 24
HOFs under light: Relevance to photon-based science and applications 光下的hof:与光子科学及其应用的相关性
IF 13.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2021-06-01 DOI: 10.1016/j.jphotochemrev.2021.100418

Hydrogen-bonded Organic Frameworks (HOFs) are an appealing, newly emerging classes of porous materials whose bright potential as multifunctional resources is reflected in important applications like gas storage and separation, molecular recognition, electric and optical materials, chemical sensing, catalysis, and biomedicine. HOFs are assembled from organic building blocks through H-bonding interactions. The resultant framework can be further reinforced via weak connections such as π-π, van der Waals, and/or C-H-π interactions. The highly flexible and reversible HOF structures are exceptionally suitable for the realization of smart HOF materials. To this end, it is crucial to unravel and control the photobehavior of these compounds at intimate levels by the use of advanced laser-based spectroscopy and microscopy techniques. The use of light to study the photophysical processes of HOF-based systems will help to trigger further research to expand their applicability in the related fields. This Review surveys the past-10-years contributions on the spectroscopy and photoinduced fast/ultrafast dynamics of HOFs, the interactions between their building units, the effect of light on their photostability, and most important photonic applications. The aim of this work is to give a rich up-to-date summary of photochemistry and related applications of HOFs and their composites. The reviewed HOFs have been divided into different families based on the nature of the linker, with the purpose of offering to the reader a concise understanding of the related photoinduced processes within each family. The relevant applications of HOFs are also briefly summarized to validate their potential use in modern science and technology.

氢键有机框架(HOFs)是一类极具吸引力的新兴多孔材料,在气体储存与分离、分子识别、光电材料、化学传感、催化和生物医学等重要应用领域具有广阔的应用前景。hof是通过氢键相互作用由有机构建块组装而成的。通过弱连接,如π-π、范德华和/或C-H-π相互作用,所得到的框架可以进一步加强。高柔性、高可逆的HOF结构特别适合实现智能HOF材料。为此,利用先进的基于激光的光谱学和显微镜技术来揭示和控制这些化合物在亲密水平上的光行为是至关重要的。利用光来研究基于hof的系统的光物理过程将有助于引发进一步的研究,以扩大其在相关领域的适用性。本文综述了近10年来在光谱学和光致快/超快动力学、其结构单元之间的相互作用、光对其光稳定性的影响以及最重要的光子应用方面的贡献。本工作的目的是提供一个丰富的最新总结光化学和相关应用的霍夫及其复合材料。所述的hof根据连接体的性质被分为不同的家族,目的是为读者提供每个家族中相关光诱导过程的简明理解。本文还简要总结了高通量通量的相关应用,以验证其在现代科学技术中的潜在应用。
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引用次数: 25
IFC(EDITORIAL BOARD) 国际金融公司(编辑部)
IF 13.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2021-06-01 DOI: 10.1016/S1389-5567(21)00024-1
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引用次数: 0
Concepts of photochemical damage of Photosystem II and the role of excessive excitation 光系统II光化学损伤的概念及过度兴奋的作用
IF 13.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2021-06-01 DOI: 10.1016/j.jphotochemrev.2021.100421

Photoinhibition is one of the most controversial topics in photophysiology. Well into the 21 st century, scientists have not agreed on the mechanism of action, primary site, and roles of excess energy absorbed by photosynthetic pigments. It is recognized that Photosystem II is the most fragile component during photoinhibition and that excess excitation absorbed by the photosynthetic pigments has a strong impact on it. Consensus is yet to come on terminology, guidelines to study photoinhibition, or boundaries of what can be considered photodamage. Some of these controversies are the result of how we understand the phenomenon of photoinhibition, as this is what determines a given experimental design. Thus, how we understand photodamage depends on the philosophical approach of each group. While some efforts have been made in the parametrization of Photosystem II photoinhibition, an updated review about the concepts of photoinhibition of Photosystem II and how to study it is still pending. In this work, a review of the concepts used in the field of photoinhibition is presented, accompanied by a synopsis on the history and mechanisms of action.

光抑制是光生理学中最具争议的话题之一。直到21 21世纪,科学家们还没有就光合色素吸收多余能量的作用机制、主要部位和作用达成一致。人们认识到光系统II是光抑制过程中最脆弱的组成部分,光合色素吸收的过量激发对其有强烈的影响。关于术语、研究光抑制的指导方针,或者什么可以被认为是光损伤的界限,尚未达成共识。其中一些争议是我们如何理解光抑制现象的结果,因为这是决定给定实验设计的因素。因此,我们如何理解光损伤取决于每个小组的哲学方法。虽然在光系统II光抑制的参数化方面做了一些努力,但对光系统II光抑制的概念和如何研究仍有待更新的综述。在这项工作中,回顾了在光抑制领域中使用的概念,并简要介绍了光抑制的历史和作用机制。
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引用次数: 24
NIR light-responsive nanocarriers for controlled release 可控释放的近红外光响应纳米载体
IF 13.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2021-06-01 DOI: 10.1016/j.jphotochemrev.2021.100420

The near-infrared (NIR) light in the wavelength range of 780−1700 nm is regarded as transparency therapeutic window for light-activated delivery system in vivo due to the deep tissue penetration and minimum cellular damage of it. Numerous reports about NIR light-sensitive nanocarriers have emerged in the past few years. Here, strategies for the design and fabrication of nanocarriers for NIR light-controlled release are reviewed, which are based on three triggering mechanisms: (1) photoreactions of chromophores, including NIR light-induced photoreactions and upconversion nanoparticles (UCNPs)-mediated photochemical reactions; (2) photothermal effect, triggered by inorganic or organic photothermal conversion agents (PCAs) with the excitation of NIR light; (3) photo-oxidation, induced by reactive oxygen species (ROS) generated by photosensitizers under NIR light radiation. Finally, the challenges and perspectives of NIR light-sensitive nanocarriers for future development are given.

780 ~ 1700 nm波长范围内的近红外(NIR)由于其穿透组织深层和细胞损伤最小,被认为是光激活给药系统在体内的透明治疗窗口。在过去的几年里,关于近红外光敏纳米载体的报道层出不穷。本文综述了基于三种触发机制的近红外光控释纳米载体的设计和制造策略:(1)发色团的光反应,包括近红外光诱导的光反应和上转化纳米颗粒(UCNPs)介导的光化学反应;(2)由无机或有机光热转换剂(PCAs)在近红外光激发下引发的光热效应;(3)近红外光辐射下光敏剂产生活性氧(ROS)诱导的光氧化。最后,对近红外光敏纳米载体的未来发展提出了挑战和展望。
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引用次数: 28
Photogenerated electrophilic radicals for the umpolung of enolate chemistry 烯酸酯化学中光生亲电自由基的研究
IF 13.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2021-03-01 DOI: 10.1016/j.jphotochemrev.2020.100387

The use of enolate chemistry is the election choice when a CC bond formation is required exploiting the acidity of carbonyl derivatives in the α position. However, a reversed-polarity equivalent of enolate chemistry is emerging making use of electrophilic radicals having a radical site in place of a negative charge in the same α position. Visible light photoredox catalysis is becoming the ideal tool for the generation of these radicals thus allowing their wide application in several synthetic routes. Aim of this review is to collect recent examples of the chemistry of photogenerated electrophilic radicals for the forging of new CC or other CY bonds.

当需要利用α位置羰基衍生物的酸性形成CC键时,使用烯醇酯化学是一种选择。然而,一种相反极性的烯醇酸化学正在出现,利用亲电自由基在相同的α位置上具有一个自由基位点代替负电荷。可见光光氧化还原催化正在成为生成这些自由基的理想工具,从而使它们在几种合成路线中得到广泛应用。本综述的目的是收集最近的例子,光产生的亲电自由基的化学锻造新的CC或其他CY键。
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引用次数: 5
Comprehensive review of photophysical parameters (ε, Φf, τs) of tetraphenylporphyrin (H2TPP) and zinc tetraphenylporphyrin (ZnTPP) – Critical benchmark molecules in photochemistry and photosynthesis 四苯基卟啉(H2TPP)和四苯基卟啉锌(ZnTPP)的光物理参数ε, Φf, τs的综合研究
IF 13.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2021-03-01 DOI: 10.1016/j.jphotochemrev.2020.100401

Tetraphenylporphyrin (H2TPP) and zinc tetraphenylporphyrin (ZnTPP) are widely used benchmark molecules in diverse photochemical studies given facile synthetic access, rich visible-region spectra, and broad structural analogy to chlorophylls. Yet the literature values for each key photophysical parameter – the molar absorption coefficient (ε), fluorescence quantum yield (Φf), and also singlet excited-state lifetime (τS) – vary over an astonishing range. Here, a comprehensive literature review (∼1940–September 2020) encompassing 871 publications is reported for these essential parameters. Each parameter is determined by measurement with distinct instrumentation and suffers idiosyncratic sources of error. The best values for H2TPP are ε = 460,000 cm−1·M−1, Φf = 0.090, and τS = 12.8 ns in Ar- purged toluene (Φf = 0.070, τS = 9.9 ns in toluene in air); the best values for ZnTPP are ε = 560,000 cm−1·M−1, Φf = 0.030, and τS = 2.1 ns in Ar-purged toluene (Φf = 0.029, τS = 2.0 ns in toluene in air). The choice of values for such parameters has far-reaching consequences in photochemistry ranging from fluorescence (or Förster) resonance energy transfer (FRET) processes to assessments of molecular brightness.

四苯基卟啉(H2TPP)和四苯基卟啉锌(ZnTPP)具有易于合成、丰富的可见区光谱和与叶绿素广泛的结构相似性,是广泛应用于各种光化学研究的基准分子。然而,每个关键的光物理参数——摩尔吸收系数(ε)、荧光量子产率(Φf)和单线态激发态寿命(τS)——的文献值在一个惊人的范围内变化。本文对这些基本参数进行了全面的文献综述(~ 1940 - 2020年9月),其中包括871篇出版物。每个参数都是通过不同的仪器测量确定的,并遭受特殊的误差来源。H2TPP的最佳值ε = 460000厘米−1·M−1,Φ0.090 f = 和τS = 12.8 ns Ar -净化甲苯(Φ0.070 f = ,τS = 9.9在空气中甲苯 ns);ZnTPP的最佳值ε = 560000厘米−1·M−1,Φ0.030 f = 和τS = 2.1 ns Ar-purged甲苯(Φ0.029 f = ,τS = 2.0  ns甲苯在空气中)。这些参数值的选择在光化学中具有深远的影响,从荧光(或Förster)共振能量转移(FRET)过程到分子亮度的评估。
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引用次数: 70
Photocatalytic non-oxidative coupling of methane: Recent progress and future 甲烷光催化非氧化偶联研究进展及展望
IF 13.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2021-03-01 DOI: 10.1016/j.jphotochemrev.2020.100400

The importance of effectively converting methane to hydrogen and high value-added hydrocarbons chemicals is becoming more significant due to the huge resources of methane and increasing demands for chemicals. However, it is hard to convert methane into more useful hydrocarbons and hydrogen due to the enormous thermodynamic barrier, which often needs high energy and often results in catalyst deactivation and unsatisfactory product selectivity. Recently, a growing number of researches focusing on photocatalytic methane conversion under mild conditions have attracted much attention, demonstrating that photocatalytic non-oxidative coupling of methane (PNOCM) is a prospective and green method for methane conversion under mild conditions. Herein, we provide a review of the recent advance, remaining challenges, and prospects in PNOCM. Moreover, this review provides considerable guidance for rational design of efficient and stable photocatalysts towards PNOCM by theory predictions and experiment results. We hope this review can attract more attention to the important research field of energy conversion.

由于巨大的甲烷资源和不断增长的化学品需求,有效地将甲烷转化为氢和高附加值的碳氢化合物化学品变得越来越重要。然而,由于巨大的热力学屏障,甲烷很难转化为更有用的碳氢化合物和氢气,这往往需要高能量,往往导致催化剂失活和产物选择性不理想。近年来,越来越多的关于温和条件下光催化甲烷转化的研究引起了人们的关注,这表明光催化甲烷非氧化偶联(PNOCM)是一种有前景的、绿色的温和条件下甲烷转化方法。在此,我们对PNOCM的最新进展、存在的挑战和前景进行了综述。理论预测和实验结果对合理设计高效稳定的PNOCM光催化剂具有一定的指导意义。我们希望这篇综述能引起人们对能量转换这一重要研究领域的更多关注。
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引用次数: 15
IFC(EDITORIAL BOARD) 国际金融公司(编辑部)
IF 13.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2021-03-01 DOI: 10.1016/S1389-5567(21)00006-X
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引用次数: 0
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Journal of Photochemistry and Photobiology C: Photochemistry Reviews
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