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Article
| Open AccessPhoto-cycloaddition reactions of vinyldiazo compounds
Heterocycles, highly prized by the pharmaceutical industry, are often constructed from diazo compounds. Here, the authors report that direct photolysis of vinyldiazo compounds followed by [3+2]-cycloaddition gives access to these motifs.
- Ming Bao
- , Klaudia Łuczak
- & Michael P. Doyle
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Article
| Open AccessCatalytic asymmetric [4 + 2] dearomative photocycloadditions of anthracene and its derivatives with alkenylazaarenes
While significant progress has been made in classical Diels-Alder reactions, the use of simple and inert feedstock chemicals under mild reaction conditions still remains challenging. Here the authors present the development of catalytic asymmetric [4 + 2] dearomative photocycloaddition involving anthracene and its derivatives with alkenylazaarenes.
- Dong Tian
- , Wenshuo Shi
- & Zhiyong Jiang
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Article
| Open AccessUnusual facet and co-catalyst effects in TiO2-based photocatalytic coupling of methane
Designing photocatalysts to enhance the efficiency of non-oxidative coupling of methane is a challenging task. Here, the authors report that the anatase TiO2 with exposed {101} facets and Pd co-catalyst enables efficient and selective methane coupling to ethane via a heterogeneous-homogeneous hybrid reaction pathway.
- Huizhen Zhang
- , Pengfei Sun
- & Ye Wang
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Article
| Open AccessIn-situ noncovalent interaction of ammonium ion enabled C–H bond functionalization of polyethylene glycols
The noncovalent interaction of ammonium ion with multidentate oxygen-based host serving as a key reacting center in catalytic reactions is rare. In this work, the authors report a noncovalent interaction of ammonium ion enabled reactivity enhancement process, achieving the C–H functionalization of polyethylene glycols with acrylates.
- Zongnan Zhang
- , Xueli Lv
- & Rong Zeng
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Article
| Open AccessDiastereoselective dearomatization of indoles via photocatalytic hydroboration on hydramine-functionalized carbon nitride
Dearomative hydroboration of predominantly existing indole derivatives provides a straightforward strategy to synthesize boryl indolines, but developing eco-friendly methods for remains challenging. Here, the authors develop a method for heterogeneous photocatalytic trans-hydroboration of indole derivatives with NHC-borane.
- Qiao Zhang
- , Wengang Xu
- & Mingbo Wu
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Article
| Open AccessAsymmetric C–H Dehydrogenative Alkenylation via a Photo-induced Chiral α‑Imino Radical Intermediate
The direct alkenylation with simple alkenes stands out as the most ideal yet challenging strategy for obtaining high-valued desaturated alkanes. Herein, the authors present a direct asymmetric dehydrogenative α-C(sp3)-H alkenylation of carbonyls based on synergistic photoredox-cobalt-chiral primary amine catalysis under visible light.
- Zongbin Jia
- , Liang Cheng
- & Sanzhong Luo
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Article
| Open AccessRapid and scalable photocatalytic C(sp2)–C(sp3) Suzuki−Miyaura cross-coupling of aryl bromides with alkyl boranes
In recent years a growing demand for drug design approaches that incorporate a higher number of sp3-hybridized carbons fuelled the development of innovative cross-coupling strategies to reliably introduce aliphatic fragments. Here, the authors present a powerful approach for the light-mediated B-alkyl Suzuki−Miyaura crosscoupling between alkyl boranes and aryl bromides.
- Ting Wan
- , Luca Capaldo
- & Timothy Noël
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Article
| Open AccessCorrelating activities and defects in (photo)electrocatalysts using in-situ multi-modal microscopic imaging
Physicochemical heterogeneity poses a significant constraint in photocatalyst advancement. Here the authors introduce a multimodal optical microscopy platform to assess activity and defects concurrently in photoelectrocatalysts, revealing that disorder can unexpectedly enhance local photoelectrocatalytic performance in certain instances.
- Camilo A. Mesa
- , Michael Sachs
- & Raj Pandya
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Article
| Open Access“On-Water” accelerated dearomative cycloaddition via aquaphotocatalysis
Developing water compatible synthetic methods for Sulfur(VI) fluoride exchange (SuFEx) chemistry is of paramount importance. Here the authors demonstrate a catalytic dearomative [2+2] photocycloaddition that significantly speeds up the synthesis of heterocyclic alkyl SuFEx hubs, leveraging the unique reactivity at the water-oil interface.
- Soo Bok Kim
- , Dong Hyeon Kim
- & Han Yong Bae
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Article
| Open AccessDinuclear gold-catalyzed divergent dechlorinative radical borylation of gem-dichloroalkanes
The widespread use of organoboronic acids has prompted the development of synthetic methodologies to meet the demands on structural diversity and functional group tolerance. Herein, the authors disclose a divergent radical dechloroborylation reaction enabled by dinuclear gold catalysis with visible light irradiation.
- Cheng-Long Ji
- , Hongliang Chen
- & Jin Xie
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Article
| Open AccessEmbedding biocatalysts in a redox polymer enhances the performance of dye-sensitized photocathodes in bias-free photoelectrochemical water splitting
A robust and efficient dye-sensitized NiO bio-hybrid photocathode based on a redox polymer and [FeFe]- hydrogenase has been developed to couple with a BiVO4 photoanode for water splitting without applied bias.
- Fangwen Cheng
- , Olha Pavliuk
- & Haining Tian
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Article
| Open AccessEnhancing photocatalytic H2O2 production with Au co-catalysts through electronic structure modification
Photocatalytic H2O2 production using Au is hindered by its inherently weak O2 adsorption. Herein, the authors modify the electronic structure of Au with MoSx to form electron deficient Au sites to promote O2 adsorption and H2O2 production.
- Xidong Zhang
- , Duoduo Gao
- & Huogen Yu
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Article
| Open AccessUltraviolet light blocking optically clear adhesives for foldable displays via highly efficient visible-light curing
The slow curing speed of UV-based methods to produce UV-blocking optically clear adhesive (OCA) for display panels poses a barrier to commercialization. Here, authors introduce a visible-light driven photo-initiating system for rapid production of OCAs, demonstrating efficient UV-blocking ability.
- Yonghwan Kwon
- , Seokju Lee
- & Min Sang Kwon
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Article
| Open AccessUltrastable halide perovskite CsPbBr3 photoanodes achieved with electrocatalytic glassy-carbon and boron-doped diamond sheets
Perovskites are desirable for photoelectrochemical applications but are unstable in aqueous electrolytes. Here, the authors report a perovskite photoanode in aqueous electrolyte, preserving 95% photocurrent density after over 100 h of operation.
- Zhonghui Zhu
- , Matyas Daboczi
- & Salvador Eslava
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Article
| Open AccessRoom temperature 3D carbon microprinting
Three-dimensional carbon microstructures with ultra-high aspect ratios are grown with a facile process using a metal-free catalyst and low-power visible light at room temperature, unlocking applications in flexible sensors and beyond.
- Fernand E. Torres-Davila
- , Katerina L. Chagoya
- & Laurene Tetard
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Article
| Open AccessBioorthogonal photocatalytic proximity labeling in primary living samples
Studying subcellular proteomes in primary living cells is crucial for understanding health and disease. Here, the authors introduce CAT-S, a non-genetic method based on photocatalysis, enabling in situ deciphering of mitochondrial proteomes in primary cells from mouse tissues and human blood.
- Ziqi Liu
- , Fuhu Guo
- & Xinyuan Fan
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Article
| Open AccessKeto-anthraquinone covalent organic framework for H2O2 photosynthesis with oxygen and alkaline water
Hydrogen peroxide photosynthesis is an important reaction that suffers from poor activity due to the high energy barrier of hydrogen extraction in water. Here, we report a keto-form anthraquinone framework that shows promising performance in alkaline conditions.
- Xiangcheng Zhang
- , Silian Cheng
- & Lizhi Zhang
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Article
| Open AccessSolar-driven sugar production directly from CO2 via a customizable electrocatalytic–biocatalytic flow system
Solar-driven artificial food synthesis from CO2 provides an approach to overcome the limitations of natural photosynthesis, but it is very challenging. Here, the authors report a hybrid electrocatalytic-biocatalytic flow system, coupling photovoltaics-powered electrocatalysis (CO2 to formate) with a five enzyme cascade platform (formate to sugar), which achieves conversion of CO2 to C6 sugar (L-sorbose) with a solar-to-food energy conversion efficiency of 3.5%.
- Guangyu Liu
- , Yuan Zhong
- & Yujie Xiong
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Article
| Open AccessInduced dipole moments in amorphous ZnCdS catalysts facilitate photocatalytic H2 evolution
The rapid recombination of photogenerated charge carriers is a key challenge for photocatalytic hydrogen production. Here, the authors report an amorphous ZnCdS to break the symmetry of atom arrangement that induces strong dipole fields, thus providing extra driving forces for charge separation.
- Xin Wang
- , Boyan Liu
- & Songcan Wang
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Review Article
| Open AccessLight-driven polymer recycling to monomers and small molecules
Chemical recycling of plastic enables renewed production of pristine materials, but generally comes at a high energy cost. This review focuses on light-driven approaches for chemically recycling and upcycling plastic waste, with emphasis on reduced energy consumption and selective transformations of challenging to recycle backbone structures.
- Laura Wimberger
- , Gervase Ng
- & Cyrille Boyer
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Article
| Open AccessPhoto-induced intramolecular dearomative [5 + 4] cycloaddition of arenes for the construction of highly strained medium-sized-rings
Medium-sized-ring compounds are challenging synthetic targets in organic chemistry. Here the authors report an intramolecular dearomative [5 + 4] cycloaddition of naphthalene-derived vinylcyclopropanes to construct these molecules under visible-light irradiation and a proper triplet photosensitizer.
- Min Zhu
- , Yuan-Jun Gao
- & Shu-Li You
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Article
| Open AccessWell-defined diatomic catalysis for photosynthesis of C2H4 from CO2
Principal interest lies in diatomic catalysts (DACs) for efficient CO2 to C2H4 photoconversion yet optimizing catalytic performance and exploring reaction mechanisms are impeded by heteronuclear atom random distribution. Here, a novel up-bottom ion-cutting architecture is proposed for fabricating well-defined DACs.
- Zhongkai Xie
- , Shengjie Xu
- & Shuyan Song
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Article
| Open AccessBubble-water/catalyst triphase interface microenvironment accelerates photocatalytic OER via optimizing semi-hydrophobic OH radical
Temperature has demonstrated the potential to regulate the photocatalytic oxygen evolution reaction (OER). This study confirms that the temperature-induced bubble-water/catalyst triphase interface microenvironment significantly enhances OER by optimizing the formation and deprotonation of semi-hydrophobic OH radicals.
- Guanhua Ren
- , Min Zhou
- & Haifeng Wang
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Article
| Open AccessSupramolecular catalyst with [FeCl4] unit boosting photoelectrochemical seawater splitting via water nucleophilic attack pathway
The strongly coupled interface between molecular catalysts and light absorbers is the key to solving efficient photoelectrochemical water oxidation. An in situ polymerized supramolecular-like catalyst was used to couple with BiVO4 for efficient and stable photoelectrochemical seawater splitting
- Jiaming Miao
- , Cheng Lin
- & Kan Zhang
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Article
| Open AccessDioxygen compatible electron donor-acceptor catalytic system and its enabled aerobic oxygenation
The photochemical properties of Electron Donor-Acceptor (EDA) complexes present exciting opportunities, but often require an inert atmosphere to maintain high efficiency. Here, the authors develop a photocatalytic system through rational design, which overcomes the oxygen-sensitive limitation of traditional EDA photocatalytic systems.
- Jialiang Wei
- , Junhong Meng
- & Ning Jiao
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Article
| Open AccessTuning light-driven oxidation of styrene inside water-soluble nanocages
Selective functionalization of C(sp2)–H bonds under ambient conditions is a persistent synthetic challenge in organic chemistry. Here the authors combine host-guest charge-transfer-based photoredox chemistry with supramolecular nano-confinement to achieve selective carbonylation of styrene by tuning the dioxygen concentration.
- Souvik Ghosal
- , Ankita Das
- & Jyotishman Dasgupta
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Article
| Open AccessLiquid metal-embraced photoactive films for artificial photosynthesis
The practical applications of photoelectrochemical water splitting pivot on significant advances that enable scalable production of robust photoactive films. Here, the authors propose a proof-of-concept for fabricating bioinspired robust photoactive films by a particle implanting technique, which embeds semiconductor photoabsorbers in the liquid metal.
- Chao Zhen
- , Xiangtao Chen
- & Gang Liu
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Article
| Open AccessMetal-free photocatalytic cross-electrophile coupling enables C1 homologation and alkylation of carboxylic acids with aldehydes
Enhancing the sp3-hybridized character of molecular structures in drug discovery is paramount. Here, the authors introduce a deoxygenative cross-electrophile coupling technique that pairs easily accessible carboxylic acid-derived redox-active esters with aldehyde sulfonyl hydrazones, employing Eosin Y as an organophotocatalyst under visible light irradiation.
- Stefano Bonciolini
- , Antonio Pulcinella
- & Timothy Noël
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Article
| Open AccessStable water splitting using photoelectrodes with a cryogelated overlayer
Photoelectrodes made of earth-abundant materials can contribute to low-cost and carbon-free hydrogen production, but suffer from a short lifetime. Here the authors report cryogel overlayer to increase the operation time of the device by regulating evolving hydrogen bubble dynamics.
- Byungjun Kang
- , Jeiwan Tan
- & Hyungsuk Lee
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Review Article
| Open AccessChallenges and recent advancements in the synthesis of α,α-disubstituted α-amino acids
α,α-Disubstituted α-amino acids (α-AAs) have improved properties compared to other amino acids. Here, the authors provide an overview of the recent advancements since 2015 and discuss existing challenges for their synthesis.
- Yu Zhang
- , Jaro Vanderghinste
- & Shoubhik Das
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Article
| Open AccessElucidation of the role of metals in the adsorption and photodegradation of herbicides by metal-organic frameworks
In this study, the authors explored the correlation between the structure and optoelectronic properties of metal organic frameworks for the removal of a harmful herbicide from water.
- Nan Chieh Chiu
- , Jacob M. Lessard
- & Kyriakos C. Stylianou
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Article
| Open AccessAccessing ladder-shape azetidine-fused indoline pentacycles through intermolecular regiodivergent aza-Paternò–Büchi reactions
Conformationally rigid 3D molecules are of high interest. Here the authors develop intermolecular aza-Paternò-Büchi reactions to access ladder-shape azetidine-fused indoline pentacycles with excellent regiodivergency and stereoselectivity.
- Jianjian Huang
- , Tai-Ping Zhou
- & Fangrui Zhong
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Article
| Open AccessCharacterization of A π–π stacking cocrystal of 4-nitrophthalonitrile directed toward application in photocatalysis
Photoexcitation of the electron-donor-acceptor (EDA) complexes are an effective approach to achieve radicals by triggering electron transfer but the catalytic version of EDA complex photoactivation remains underdeveloped. Here, the authors introduce 4-nitrophthalonitrile as an electron acceptor to facilitate π-stacking with electron-rich aromatics to form EDA complexes.
- Ting Xue
- , Cheng Ma
- & Rong Zeng
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Article
| Open AccessIn-situ formatting donor-acceptor polymer with giant dipole moment and ultrafast exciton separation
Donor-acceptor polymers have potential for application in photocatalysis, but often harsh synthetic conditions are required. Here, the authors report a post-synthetic method for conversion to donor-acceptor states, to give a polymer capable of enhancing photocatalytic hydrogen peroxide synthesis.
- Chang Cheng
- , Jiaguo Yu
- & Mietek Jaroniec
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Article
| Open AccessA nonmetallic plasmonic catalyst for photothermal CO2 flow conversion with high activity, selectivity and durability
In this work, the authors design a Mo2N/MoO2-x nonmetallic plasmonic catalyst by regulating synergy between two specific active sites. Highly efficient, selective, and durable CO2 hydrogenation under relatively mild reaction conditions is achieved
- Xueying Wan
- , Yifan Li
- & Yujie Xiong
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Article
| Open AccessAg3PO4 enables the generation of long-lived radical cations for visible light-driven [2 + 2] and [4 + 2] pericyclic reactions
Photoredox catalysis is an important approach for synthesizing fine chemicals from olefins, but the limited lifetime of radical cation intermediates severely restricts the efficiency. Here, the authors report that Ag3PO4 can efficiently catalyze intramolecular and intermolecular [2 + 2] and Diels–Alder cycloadditions under visible-light irradiation.
- Lirong Guo
- , Rongchen Chu
- & Yifeng Wang
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Article
| Open AccessPhotocatalytic ethylene production by oxidative dehydrogenation of ethane with dioxygen on ZnO-supported PdZn intermetallic nanoparticles
The selective oxidative dehydrogenation of ethane is attracting increasing attention as a method for ethylene production. Here, PdZn supported on ZnO affords record-breaking photocatalytic ethane-to-ethylene conversion rate, emphasizing the pivotal role of the interface between PdZn and ZnO in the process.
- Pu Wang
- , Xingyu Zhang
- & Tierui Zhang
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Article
| Open AccessPt-doped Ru nanoparticles loaded on ‘black gold’ plasmonic nanoreactors as air stable reduction catalysts
An air-stable plasmonic catalyst using Pt-Ru on black gold achieves 90% selectivity in acetylene semi-hydrogenation using plasmonic photochemistry. Mechanistic experiments highlight the role of non-thermal and thermal effects for this reaction.
- Gunjan Sharma
- , Rishi Verma
- & Vivek Polshettiwar
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Article
| Open AccessOvercoming small-bandgap charge recombination in visible and NIR-light-driven hydrogen evolution by engineering the polymer photocatalyst structure
Designing an organic polymer photocatalyst for efficient hydrogen evolution in the near-infrared (NIR) light region is still a major challenge. The authors present here a series of polymer nanoparticles for a efficient hydrogen evolution under visible and NIR light irradiation, without combining or hybridizing with other materials.
- Mohamed Hammad Elsayed
- , Mohamed Abdellah
- & Ho-Hsiu Chou
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Article
| Open AccessElectrophotocatalytic hydrogenation of imines and reductive functionalization of aryl halides
Open-shell catalytically active species are widely used in energy-consuming redox reactions, but their excited-state lifetimes are usually short. Here, the authors report a closed-shell thioxanthone-hydrogen anion species generated under electrochemical conditions, which can be photochemically converted to a potent and long-lived reductant.
- Wen-Jie Kang
- , Yanbin Zhang
- & Hao Guo
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Article
| Open AccessPhotocatalytic aerobic oxidation of C(sp3)-H bonds
The authors report a family of photocatalysts containing Ce active sites and perylene diimide ligands for the aerobic oxidation of substituted toluene, ethylbenzene, benzyl alcohol, thioanisole, and benzylamine in acetonitrile.
- Lei Zhang
- , Run-Han Li
- & Ya-Qian Lan
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Article
| Open AccessPhotogenerated outer electric field induced electrophoresis of organic nanocrystals for effective solid-solid photocatalysis
Charge accumulation in organic photocatalysts leads to an overlooked macroscopic particle migration, crucial for heterogeneous photocatalytic kinetics. Authors demonstrate self-driven electrophoresis of organic nanocrystals via rationally designed photogenerated outer electric field (OEF).
- Yan Guo
- , Bowen Zhu
- & Yongfa Zhu
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Article
| Open AccessElucidating protonation pathways in CO2 photoreduction using the kinetic isotope effect
Yin et al. reveal a protonation pathway in CO2 photoreduction on TiO2, challenging electron activation theories and diversifying photocatalyst design, distinct from Fischer-Tropsch and Sabatier processes.
- Shikang Yin
- , Yiying Zhou
- & Pengwei Huo
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Article
| Open AccessDual-plasmonic Au@Cu7S4 yolk@shell nanocrystals for photocatalytic hydrogen production across visible to near infrared spectral region
Near infrared energy remains untapped toward the maneuvering of entire solar spectrum harvesting for fulfilling nuts and bolts of solar hydrogen production. Here, the authors report the use of Au@Cu7S4 yolk@shell nanocrystals for hydrogen production from untapped near infrared energy.
- Chun-Wen Tsao
- , Sudhakar Narra
- & Yung-Jung Hsu
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Article
| Open AccessEfficient and stable visible-light-driven Z-scheme overall water splitting using an oxysulfide H2 evolution photocatalyst
Photocatalytic water splitting systems using Sm2Ti2O5S2, a visible light-active oxysulfide, exhibited low efficiencies due to low intrinsic photoactivity and rapid back reaction. Here, the efficiency was greatly improved by refining the preparation of photocatalysts and electron mediators
- Lihua Lin
- , Yiwen Ma
- & Kazunari Domen
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Article
| Open AccessLarge electronegativity differences between adjacent atomic sites activate and stabilize ZnIn2S4 for efficient photocatalytic overall water splitting
Solving component homogeneity and sulfur instability of metal sulfides is crucial for photocatalytic overall water splitting. Here, the authors develop a distortion evoked cation site oxygen doping to create electronegativity differences between adjacent atom and enhance photocatalytic activity
- Xu Xin
- , Yuke Li
- & Xuanhua Li
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Comment
| Open AccessImproving reproducibility of photocatalytic reactions—how to facilitate broad application of new methods
Photocatalysis, as a powerful tool for synthetic transformations, has the potential to impact industrial applications. In this commentary, we discuss the challenges and requirements with respect to reproducing published photocatalytic reactions in the (life science) industry.
- Santiago Cañellas
- , Manuel Nuño
- & Elisabeth Speckmeier
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Article
| Open AccessOne-dimensional single atom arrays on ferroelectric nanosheets for enhanced CO2 photoreduction
The authors report a study preparing single atom (M = Pt, Ag, Fe, Co, and Ni) arrays on Au/Bi4Ti3O12 nanosheets using electric field polarization techniques. Photocatalytic CO2 reduction is shown to proceed effectively over Au/Bi4Ti3O12.
- Lizhen Liu
- , Jingcong Hu
- & Hongwei Huang
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Article
| Open AccessUnderstanding the light induced hydrophilicity of metal-oxide thin films
Light-induced hydrophilicity of TiO2 and ZnO surfaces rely on the same physics and involve excitation of electron-hole pairs. Here, the authors propose and test a model for the photowetting of TiO2 and ZnO thin films. The results suggest design rules for materials exhibiting photocatalytic wetting.
- Rucha Anil Deshpande
- , Jesper Navne
- & Rafael Taboryski