Article
Chemistry, Inorganic & Nuclear
Yang Cheng, Qingqing Yang, Jiang He, Wenjie Zou, Keyu Liao, Xiaoyong Chang, Chao Zou, Wei Lu
Summary: This article introduces a series of substituted anionic ligands containing Cr(iii) complexes, which exhibit phosphorescent properties in degassed fluid solutions.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Physical
Tobias Morack, Carina Onneken, Hiroshi Nakakohara, Christian Mueck-Lichtenfeld, Ryan Gilmour
Summary: Researchers have developed a platform for enantioselective prenylation using light, aiming to facilitate chiral drug discovery. Detailed mechanistic analysis has led to the development of an efficient method for preparing enantioselective variants. The chiral pool quasi-enantiomers quinine and quinidine play an important role as catalysts in this process.
Article
Chemistry, Physical
Steven Sittel, Arne Christian Sell, Kamil Hofmann, Christina Wiedemann, Jan Philipp Nau, Christoph Kerzig, Georg Manolikakes, Katja Heinze
Summary: In this study, a photocatalytic approach using sensitizers made from earth-abundant chromium(III) ions and visible light was employed to incorporate sulfur dioxide into organic compounds, leading to the formation of sulfones and sulfonamides. Three different chromium(III) sensitizers were used, and their reactivity and stability under the reaction conditions were investigated. Through various experiments, the key reaction steps and challenges in these transformations were identified, and the reactivity of the reduced chromium complex was found to be a crucial factor determining the reaction outcomes.
Article
Chemistry, Multidisciplinary
Monochura Saha, Munshi Sahid Hossain, Subhajit Bandyopadhyay
Summary: This study presents a PLP-photoswitch-imidazole triad that allows the racemization reaction of amino acids to be controlled by light, by adjusting the distance between the basic residue and the reaction center.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Amir Abbas, Eva Oswald, Jan Romer, Anja Lenzer, Magdalena Heiland, Carsten Streb, Christine Kranz, Andrea Pannwitz
Summary: Nature utilizes reactive components in biological membranes for light-driven photosynthesis. A model artificial photosynthetic system for light-driven hydrogen (H-2) evolution based on liposomes has been developed, with DMPC showing increased catalytic activity compared to other lipid matrixes. In situ scanning electrochemical microscopy measurements reveal an activation mechanism induced by the fluid-gel phase transition of DMPC.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Jakub Durka, Joanna Turkowska, Dorota Gryko
Summary: Diazo compounds are valuable reagents in organic synthesis, and their photochemical reactions under visible light irradiation offer sustainable and efficient alternatives to transition metal catalysis. These reactions have shown promising applications in various transformations, highlighting a potential future direction for greener synthetic methodologies.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2021)
Article
Chemistry, Multidisciplinary
Peter Goedtel, Jessica Starrett, Zbigniew L. Pianowski
Summary: Hemipiperazines, a newly discovered class of peptide-derived molecular photoswitches, show high biocompatibility and therapeutic potential. In this study, we investigate the photochromism of heterocyclic hemipiperazines for the first time. They exhibit long thermal lifetimes and expanded band separation between photoisomers. Efficient photoisomerization is achieved under aqueous conditions with the addition of organic co-solvent. Bidirectional switching with visible light is observed in an extended aromatic system.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Rui Guo, Haijing Xiao, Sijia Li, Yixin Luo, Jiahui Bai, Mengzhen Zhang, Yinlong Guo, Xiaotian Qi, Guozhu Zhang
Summary: This study successfully developed a mild and general method for C(sp(3))-H functionalization of cyclic amines. By utilizing intramolecular 1,5-hydrogen atom transfer (HAT) under photo-irradiation, the enantioselective C(sp(3))-H alkynylation of unactivated cyclic 2-iodo-benzamide was achieved. The use of a new bisoxazoline diphenylamine ligand in combination with 1,1'-bi-2-naphthol significantly improved the reduction potential of the copper complex. This method not only demonstrates a broad substrate scope, including unprecedented benzocyclic amines, but also exhibits excellent diastereoselectivity in 2-monosubstituted cyclic amines via substrate control.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Fabien Kohl, Aaron Gerwien, Frank Hampel, Peter Mayer, Henry Dube
Summary: Molecular photoswitches that allow precise control over geometrical and electronic changes are highly sought after for the development of responsive nanosystems. In this study, a novel multiphotoswitch architecture is presented, which offers an advantageous combination of property control. The hemithioindigo-based trioxobicyclononadiene (HTI-TOND) has a rigid three-dimensional molecular structure that undergoes different rearrangement reactions upon photochemical and thermal signaling, resulting in reversible access to multiple states with distinct geometric and electronic properties.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Inorganic & Nuclear
Duna A. K. Alenazi, Huda S. AlSalem, Aliyah S. Alhawiti, Mona S. Binkadem, Abeer Abdulaziz H. Bukhari, Nahlah A. Alhadhrami, Raedah A. S. Alatawi, May Abdullah Abomuti
Summary: Lanthanide-doped strontium aluminate phosphor (LSAP) nanoparticles were synthesized and immobilized into carboxymethyl cellulose (CMC) hydrogel for fluorescent marking of fingerprints, offering potential for low costs, low environmental impact, and high scale production.
INORGANIC CHEMISTRY COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Peifeng Su, Zhe Chen, Jinyu Ni, Zhenjie Yang, Yinwu Li, Zhuofeng Ke
Summary: This study demonstrates the importance of overcoming the alkoxide trap problem and the impact of the chromium center's oxidation state on catalytic activity. By surmounting the alkoxide trap, a Cr(0) catalyst is developed for efficient C-alkylation between alcohols via borrowing hydrogen/hydrogen autotransfer. The Cr(0) catalyst shows excellent catalytic performance and can avoid the d-p p interaction, overcoming the thermodynamic sink caused by the alkoxide trap. This strategy could be helpful in developing efficient and nonprecious transition metal catalysts.
Article
Chemistry, Multidisciplinary
Tuzhi Xiong, Xincheng Yao, Zhixiao Zhu, Ran Xiao, Yu-wen Hu, Yongchao Huang, Shanqing Zhang, M. -Sadeeq (Jie Tang) Balogun
Summary: By combining interfacial engineering and elemental doping, a unique structure with high-valence non-3d metal and non-metal integration was achieved on stainless steel mesh for efficient hydrogen evolution reaction (HER) in both alkaline and acidic media, showing superior performance to commercial Pt/C catalysts.
Review
Chemistry, Multidisciplinary
Johannes Grosskopf, Thorsten Bach
Summary: Upon irradiation with a suitable chiral catalyst, racemic compounds can be converted into enantiopure compounds through a process called photochemical deracemization. This review comprehensively covers the research and current developments in this field, discussing the reactions and mechanistic details underlying the presented reaction. Photochemical deracemization offers a unique opportunity to directly obtain enantiopure compounds from racemates, and short-lived intermediates play a key role in determining the enantioselectivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Multidisciplinary Sciences
Huamin Wang, Huiling Shao, Ankita Das, Subhabrata Dutta, Hok Tsun Chan, Constantin Daniliuc, K. N. Houk, Frank Glorius
Summary: In this study, a photoinduced ring enlargement method of thiophenes was developed, which involves the insertion of bicyclo[1.1.0]butanes to form eight-membered bicyclic rings under mild conditions. The synthetic value, broad functional-group compatibility, and excellent chemo- and regioselectivity were demonstrated by scope evaluation and product derivatization. Experimental and computational studies suggested a photoredox-induced radical pathway.
Article
Biochemistry & Molecular Biology
Pier Luigi Gentili, Antonio Capaccioni, Raimondo Germani, Simona Fantacci
Summary: Photochromic compounds are utilized to develop neuron surrogates for neuromorphic engineering in wetware. The photochromic behaviors of (E)-3,4,6-trichloro-2-(p-diazenil)-phenol (t-DZH) and its conjugated phenoxide base (t-DZ) in various media have been experimentally investigated. The results suggest that t-DZH and t-DZ can serve as molecular probes and potential ingredients for implementing pacemaker neurons that communicate optically in wetware.
Article
Chemistry, Multidisciplinary
Cuncai Lv, Xianhua Bai, Shangbo Ning, Chenxi Song, Qingqing Guan, Bang Liu, Yaguang Li, Jinhua Ye
Summary: Converting CO2 into fuels or chemicals through photothermal catalysis is a promising solution for energy shortage and global warming. Understanding nanomaterial strategies in this process is crucial for device and catalyst design, as well as maximizing CO2 hydrogenation performance. This Perspective discusses nanomaterial design concepts, reviews recent progress, and highlights challenges and opportunities in photothermal CO2 hydrogenation.
Article
Chemistry, Physical
Yu Nie, Tingting Bo, Wei Zhou, Huilin Hu, Xiang Huang, Huaiyuan Wang, Xin Tan, Lequan Liu, Jinhua Ye, Tao Yu
Summary: Regulating the energy barrier of *COOH is crucial for the rate determining step in the photocatalytic reduction of CO2 to produce CO gas. In this study, an appropriate Zn vacancy on ZnIn2S4 was synthesized to enhance the photocatalytic CO2 reduction capacity (CO: 5.63 mmol g(-1) h(-1)) and selectivity (CO: 97.9%). Different sulfhydryl groups were used to regulate the formation of Zn vacancies in ZnIn2S4, leading to the generation of unsaturated sulfur coordination state adjacent to the Zn vacancy with fewer electrons compared to ZnIn2S4 without Zn vacancy. Experimental analysis and theoretical calculations demonstrated that the appropriate Zn vacancy shifted the Gibbs free energy of *COOH from endothermic to exothermic during the photoreduction of CO2. This work provides an engineering method to optimize cation vacancies and improve the efficiency of photocatalytic CO2 reduction by adjusting the energy barrier of intermediates.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Nanoscience & Nanotechnology
Wuqing Luo, An Li, Baopeng Yang, Hong Pang, Junwei Fu, Gen Chen, Min Liu, Xiaohe Liu, Renzhi Ma, Jinhua Ye, Ning Zhang
Summary: A hexagonal phase ZnS photocatalyst is synthesized and exhibits higher CO selectivity and better activity for CO2 reduction reactions compared to cubic ZnS. The study provides valuable insights into the synthesis and electronic structure of hexagonal ZnS for CO2 reduction reactions, which can inspire the design of highly active photocatalysts.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Xuelian Yu, Jian Xu, Jiangpeng Wang, Jinyu Qiu, Xiaoqiang An, Zhuan Wang, Guocheng Lv, Libing Liao, Jinhua Ye
Summary: In this study, a new protocol of natural Z-Scheme heterostructures based on red mud bauxite waste was demonstrated. The improved component and interfacial structure enabled efficient spatial separation of photo-generated carriers for overall water splitting, making it a promising photocatalyst for solar fuel production. This work presents the first Z-Scheme heterojunction based on natural minerals and provides a new avenue for the utilization of natural minerals for advanced catalysis applications.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Kang Peng, Jingying Ye, Hongjie Wang, Hui Song, Bowen Deng, Shuang Song, Yihan Wang, Linjie Zuo, Jinhua Ye
Summary: This study demonstrates that Ru nanoparticles supported on natural halloysite nanotubes can enhance the photothermal catalytic activity and selectivity of CO2 methanation under continuous flow conditions. The optimized catalyst exhibits a photothermal catalytic performance of 1704 mmolCH(4) g(cat)(-1) h(-1) with 93% CH4 selectivity and 68% CO2 conversion, surpassing other Ru-based catalysts in photothermal CO2 reduction. The excellent catalytic performance is attributed to the unique mesoporous tubular structure, efficient light-to-heat conversion, and interfacial interactions between halloysite nanotubes and Ru. This method of utilizing natural minerals as support provides a convenient approach for the rational design of abundant and low-cost catalysts for efficient photothermal catalytic CO2 reduction.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Xinmin Yang, Jiwei Cui, Xiaolu Liu, Qiqi Zhang, Defa Wang, Jinhua Ye, Lequan Liu
Summary: Cocatalyst is crucial in photocatalytic overall water splitting (POWS), but it also promotes H2-O2 recombination. In this study, a strategic approach of selectively coating single-layer graphene on metal cocatalyst was developed to suppress the backward reaction for efficient POWS. The results demonstrate the effectiveness of this method and its potential in developing cocatalysts with suppressed backward reaction for efficient POWS.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Bowen Deng, Hui Song, Qi Wang, Jianan Hong, Shuang Song, Yanwei Zhang, Kang Peng, Hongwei Zhang, Tetsuya Kako, Jinhua Ye
Summary: A Ru/In2O3 catalyst is reported for efficient and stable photothermal CH3OH production from CO2 hydrogenation under atmospheric pressure. The catalyst demonstrates a remarkable solar CH3OH production, which is more than 50 times higher than that of pure In2O3 and surpasses other reported In2O3-based photothermal catalysts. Detailed characterizations show that the interaction between Ru and In2O3 enhances the activation of CO2 and H-2, and Ru modulates the electronic structure of In2O3, promoting the generation of oxygen vacancies for CH3OH formation. This work provides a rational design approach for efficient catalysts in solar CH3OH production from CO2 hydrogenation under mild conditions.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Multidisciplinary Sciences
Yaguang Li, Xianhua Bai, Dachao Yuan, Chenyang Yu, Xingyuan San, Yunna Guo, Liqiang Zhang, Jinhua Ye
Summary: Cu-based high-entropy two-dimensional oxide is synthesized using a PVP templated method and shows enhanced sintering resistance and CO2 hydrogenation activity. It achieves a record photochemical energy conversion efficiency in photothermal CO2 hydrogenation under ambient sunlight irradiation.
NATURE COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Xin Chen, Junxiang Chen, Huayu Chen, Qiqi Zhang, Jiaxuan Li, Jiwei Cui, Yanhui Sun, Defa Wang, Jinhua Ye, Lequan Liu
Summary: In this study, a strategy of promoting water dissociation on Bi2O2CO3 is reported to achieve high solar to formate energy conversion in CO2 electroreduction. The authors identify CO3* as the key surface species for formate formation through electron spin resonance measurements and in situ Raman spectroscopy combined with isotopic labelling. The efficiency of solar to formate energy conversion reaches as high as 13.3% when combined with a photovoltaic device.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Hao Wu, Lei Zhang, Songying Qu, Aijun Du, Junwang Tang, Yun Hau Ng
Summary: Hydrogen dopants and oxygen vacancies are important in BiVO4 photoanodes, but the impact of hydrogenation on charge transport, particularly electron small polaron formation, is not well understood. This study demonstrates that mild hydrogenation of nanoporous BiVO4 reduces the charge transport barrier, as shown by thermally activating photocurrent responses. The hydrogen atoms occupy oxygen vacancies, reducing the activation energy and facilitating electron small polaron transport. A BiVO4 photoanode with NiFeOx cocatalyst achieves an applied-bias photon-to-current efficiency of 1.91% at 0.58 V vs RHE. This study expands the understanding of hydrogen doping beyond conventional donor density/surface chemisorption mediations to include small polaron hopping.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Xiaolu Liu, Xinmin Yang, Jiwei Cui, Chenhe Wu, Yanhui Sun, Xuemei Du, Junxiang Chen, Jinhua Ye, Lequan Liu
Summary: This study demonstrates the great potential of using highly stable and active Ni-based photocatalysts for photocatalytic overall water splitting (POWS). Ni nanoparticles encapsulated in a nitrogen-doped ultrathin graphene layer were found to be an active, stable, and low-cost cocatalyst for POWS. The H-2 evolution rate over this cocatalyst was significantly higher than that of typical Pt cocatalyst, and the oxidation of Ni during the reaction was effectively suppressed through N-doped graphene coating. In addition to improving charge carrier dynamics, the introduction of N reduced the apparent activation energy of POWS.
Article
Chemistry, Multidisciplinary
Hao Huang, Shengyao Wang, Xingce Fan, Davin Philo, Liping Fang, Wenguang Tu, Teng Qiu, Zhigang Zou, Jinhua Ye
Summary: Au NPs and TiO2 are integrated via a solid-state dewetting technique, and the plasmonic frequencies range from visible to NIR region. The system allows for the photofixation of N-2 to NH3 under NIR light, offering a carbon-free and sustainable strategy for NH3 production. The Au/TiO2 plasmonic photocatalyst system shows stable performance and has the potential for better utilization of solar energy for nitrogen fixation.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Applied
Hong Pang, Fumihiko Ichihara, Xianguang Meng, Lijuan Li, Yuqi Xiao, Wei Zhou, Jinhua Ye
Summary: This study investigates the influence of different transition metal ions on the photocatalytic CO2 reduction using copper-doped ZnS nanocrystals as the main catalyst. It was found that Ni2+, Co2+, and Cd2+ enhanced CO2 reduction, while Fe2+ suppressed the photocatalytic activity. The modified ZnS:Cu photocatalysts demonstrated tunable product selectivity, with Ni2+ and Co2+ showing high selectivity for syngas production and Cd2+ displaying remarkable formate selectivity.
JOURNAL OF ENERGY CHEMISTRY
(2023)
Review
Chemistry, Multidisciplinary
Bin Chang, Hong Pang, Fazal Raziq, Sibo Wang, Kuo-Wei Huang, Jinhua Ye, Huabin Zhang
Summary: In this review, the recent progress and challenges in preparing C2+ products are discussed. The recent advancements in carbon-carbon coupling results and proposed mechanisms are elaborated, along with the complex scenarios involved in the initial CO2 activation process, catalyst micro/nanostructure design, and mass transfer conditions optimization. The synergistic realization of high C2+ product selectivity through catalyst design and the influence of electrolytes using theoretical calculation analysis and machine learning prediction are also proposed. The in situ/operando techniques for tracking structural evolution and recording reaction intermediates during electrocatalysis are elaborated, as well as insights into triphasic interfacial reaction systems with improved C2+ selectivity.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Physical
Chengcheng Zhang, Yingkui Yan, Hubiao Huang, Xinsheng Peng, Hui Song, Jinhua Ye, Li Shi
Summary: Fe@PCN-222 is an efficient and selective photocatalyst that can oxidize CH4 to liquid oxygenates at room temperature using visible light. The presence of Fe single-atoms promotes the transfer of photogenerated electrons and activates H2O2, resulting in a substantial improvement in the selectivity and activity of liquid oxygenate production.
