Article
Chemistry, Multidisciplinary
Arjun Vijeta, Carla Casadevall, Souvik Roy, Erwin Reisner
Summary: Ni-deposited mesoporous graphitic carbon nitride (Ni-mpg-CNx) is introduced as an inexpensive, robust, easily synthesizable and recyclable material that functions as an integrated dual photocatalytic system. It overcomes the limitations of traditional reactions by providing new opportunities for dual catalysis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Zhenghui Wen, Ting Wan, Arjun Vijeta, Carla Casadevall, Laura Buglioni, Erwin Reisner, Timothy Noel
Summary: The mesoporous carbon nitride (mpg-CNx) photocatalyst enables efficient azolation of various arenes through direct oxidation, with a broad substrate scope and high photocatalytic stability. This method offers a greener and more sustainable route for the late-stage functionalization of pharmaceuticals.
Article
Chemistry, Physical
Chun-Yao Wang, Kazuhiko Maeda, Lee-Lee Chang, Kuo-Lun Tung, Chechia Hu
Summary: This review focuses on the synthesis and applications of carbon nitride materials. Carbon nitride is a polymer semiconductor composed of carbon and nitrogen, with graphitic carbon nitride being the most commonly synthesized form. It has a suitable bandgap energy for visible light-driven photocatalysis. The nitrogen atoms in the edges of 2D g-C3N4 nanosheets play a role in catalytic conversion reactions. The carbon/nitrogen ratio and structural features of carbon nitride are influenced by precursors and synthetic processes. The correlations between different units in C3Nx were studied to understand their structural features and activity in photocatalysis and catalysis. The review summarizes the latest synthetic approaches of CNx and discusses their potential applications in energy and environmental fields.
Article
Chemistry, Physical
Dominik Birnthaler, Rok Narobe, Eliseo Lopez-Berguno, Christoph Haag, Burkhard Koenig
Summary: Ligand-to-metal charge transfer (LMCT) photo-catalysis enables the activation and utilization of halides and other heteroatoms in metal complexes. The application of bismuth LMCT in organic radical coupling reactions has been expanded, generating chlorine and carboxyl radicals in net-oxidative and redox-neutral photochemical reactions. The study reveals BiCl4- and BiCl52- as the catalytically active bismuth species under 385 nm irradiation, providing insight into the reactivity of the highly reactive bismuth(II) catalyst fragment through cyclic voltammetry and UV-vis studies.
Article
Chemistry, Multidisciplinary
Feng Chen, Xi-Lin Wu, Chenyang Shi, Hongjun Lin, Jianrong Chen, Yanpeng Shi, Shaobin Wang, Xiaoguang Duan
Summary: A novel transition metal single-atom catalyst has been developed for efficient heterogeneous Fenton-like reactions, showing excellent cyclic stability and a wide effective pH range. The catalyst accelerates the production and separation of charge carriers, enhancing the reaction performance.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Sumin Kim, Jinsol Bok, Byoung-Hoon Lee, Hyunwoo Choi, Youngran Seo, Jiheon Kim, Junhee Kim, Wonjae Ko, Kug-Seung Lee, Sung-Pyo Cho, Taeghwan Hyeon, Dongwon Yoo
Summary: This study demonstrates the atomic site orthogonality in the M-1/C3N4 system, enabling a cascade photoredox reaction in a single system. The system utilizes visible-light-generated holes and electrons from C3N4 to drive oxidation reactions, fluorination reactions, and cross-coupling reactions.
Article
Chemistry, Physical
Yelan Xiao, Yecheng Leng, Xinxin Lu, Shun-Cheung Cheng, Hao Huang, Man-Kit Tse, Jiechun Liang, Wenguang Tu, Chi-Chiu Ko, Xi Zhu, Lu Wang, Yong Zhou, Yingfang Yao, Zhigang Zou
Summary: Photocatalytic radical fluoroalkylation is an important method to prepare organofluorine compounds. This study introduces a cost-effective and recyclable heterogeneous photocatalysis using cyano-modified graphitic carbon nitride as the photocatalyst. The photocatalytic process is attributed to the long-lived triplet excited states and the strong interaction between the catalyst and substrate. Moreover, the catalyst shows high performance, wide reaction scope, and can be easily recovered and reused for multiple catalytic cycles.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Organic
Xiao Dan, Qian Yang, Liuzhuang Xing, Yurong Tang, Wentao Wang, Yunfei Cai
Summary: A fully heterogeneous metallaphotocatalytic C-C cross-coupling of aryl/vinyl halides with alkyl/allyl trifluoroborates has been developed using an integrated bipyridyl-Ni-(II)-carbon nitride as a stable and recyclable bifunctional catalyst. This visible-light-mediated heterogeneous protocol enables the sustainable synthesis of diverse valuable diarylmethanes and allylarenes in high efficiency.
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
Zhaofei Zhang, Yangsen Xu, Qitao Zhang, Shaofan Fang, Hongli Sun, Wei Ou, Chenliang Su
Summary: A combination of copper catalysis and semiconductor photocatalysis using polymeric carbon nitride (PCN) was developed for multi-type cross-coupling reactions. This dual-catalytic system enables mild C-H arylation, chalcogenation, and C-N cross-coupling reactions under visible light irradiation with a broad substrate scope. The metal-free and low-cost PCN photocatalyst can be easily recovered and reused multiple times, showing good yields and functional group tolerance.
Article
Multidisciplinary Sciences
Liuzhuang Xing, Qian Yang, Chen Zhu, Yilian Bai, Yurong Tang, Magnus Rueping, Yunfei Cai
Summary: In this study, the authors successfully incorporated privileged homogeneous bipyridyl-based Ni-catalysts into highly ordered and crystalline potassium poly(heptazine imide) (K-PHI), achieving the development goal of heterogeneous metallaphotocatalysis. The LnNi-PHI catalysts exhibit superior chemical stability and recyclability in C-P, C-S, C-O and C-N cross-coupling reactions.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Arjun Vijeta, Carla Casadevall, Erwin Reisner
Summary: In this study, a photocatalytic protocol for the selective synthesis of primary anilines was developed using a heterogeneous photocatalyst powder consisting of nickel(II) deposited on mesoporous carbon nitride. The method showed high functional group tolerance, mild reaction conditions, and easy recovery and reuse of the photocatalyst powder.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Materials Science, Multidisciplinary
Tingting Xu, Zhonghui Xia, Hongguan Li, Ping Niu, Shulan Wang, Li Li
Summary: This study reports the construction of a crystalline g-C3N4/g-C3N4-xSx heterostructure to improve the charge separation and transfer in photocatalysts. The prepared g-C3N4/g-C3N4-xSx exhibited remarkable photocatalytic performance and superior piezocatalytic activity. The findings provide new strategies for the design of efficient polymeric photocatalysts and highlight the piezocatalytic studies of g-C3N4.
ENERGY & ENVIRONMENTAL MATERIALS
(2023)
Article
Chemistry, Physical
Zhong-Kai Xie, Yu-Jing Jia, Yuan-Yong Huang, Dong-Bo Xu, Xiao-Jie Wu, Min Chen, Wei-Dong Shi
Summary: This study designs metal-free two-dimensional graphitic carbon nitride and achieves simultaneous photocatalytic reforming of lignocellulose and water under near-infrared light irradiation. By analyzing the material, it is found that there is an intermediate band that extends the spectral absorption range and promotes the separation of photogenerated charge carriers, allowing the photocatalytic conversion of lignocellulose and hydrogen generation.
Review
Acoustics
Ingrid V. Machado, Jhonathan R. N. dos Santos, Marcelo A. P. Januario, Arlene G. Correa
Summary: By utilizing ultrasound-assisted multicomponent reactions under heterogeneous catalysis, it is possible to efficiently synthesize biologically active organic compounds with reduced costs and energy consumption.
ULTRASONICS SONOCHEMISTRY
(2021)
Review
Chemistry, Multidisciplinary
Christene A. Smith, Mina R. Narouz, Paul A. Lummis, Ishwar Singh, Ali Nazemi, Chien-Hung Li, Cathleen M. Crudden
Article
Chemistry, Inorganic & Nuclear
Ivan G. Logvinenko, Yevheniia Markushyna, Ivan S. Kondratov, Bohdan V. Vashchenko, Maria Kliachyna, Yuliya Tokaryeva, Valentyna Pivnytska, Oleksandr O. Grygorenko, Guenter Haufe
JOURNAL OF FLUORINE CHEMISTRY
(2020)
Article
Chemistry, Multidisciplinary
Aleksandr Savateev, Nadezda Tarakina, Volker Strauss, Tanveer Hussain, Katharina ten Brummelhuis, Jose Manuel Sanchez Vadillo, Yevheniia Markushyna, Stefano Mazzanti, Alexander P. Tyutyunnik, Ralf Walczak, Martin Oschatz, Dirk M. Guldi, Amir Karton, Markus Antonietti
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2020)
Article
Chemistry, Multidisciplinary
Christene Anne Smith, Vincenzo Alessandro Cataldo, Thomas Dimke, Ina Stephan, Ryan Guterman
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2020)
Article
Chemistry, Multidisciplinary
Robert M. Mayall, Christene A. Smith, Alexander S. Hyla, Dianne S. Lee, Cathleen M. Crudden, Viola Birss
Article
Chemistry, Multidisciplinary
Aleksandr Savateev, Yevheniia Markushyna, Christoph M. Schusslbauer, Tobias Ullrich, Dirk M. Guldi, Markus Antonietti
Summary: Photocatalysis involves converting small organic molecules into desired products using light responsive materials, electromagnetic radiation, and electron mediators. Substituting low molecular weight reagents with redox active functional materials can expand the utility of photocatalysis beyond organic synthesis and environmental applications. Designing hybrid nanocomposites as the base allows reversible modulation of electrical conductivity and study of photocatalytic processes mediated by semiconducting photocatalysts through electrical conductivity measurements.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Yajun Zou, Kai Xiao, Qing Qin, Jian-Wen Shi, Tobias Heil, Yevheniia Markushyna, Lei Jiang, Markus Antonietti, Aleksandr Savateev
Summary: The use of a free-standing and flow-through carbon nitride nanotube (CNN) membrane with a pore diameter of 40 nm for confined photocatalytic reactions has shown improved performance compared to bulk reactions, achieving a higher catalytic turnover frequency. This nanoconfined catalysis strategy allows for quantitatively assessing the photocatalytic performance in spatially isolated nanoreactors, providing crucial insights on catalysis in such environments and potentially gaining a fundamental understanding of complex chemical processes.
Article
Chemistry, Multidisciplinary
Yevheniia Markushyna, Christoph M. Schuesslbauer, Tobias Ullrich, Dirk M. Guldi, Markus Antonietti, Aleksandr Savateev
Summary: Photocatalysis utilizes different colors of excitation light to selectively convert S-arylthioacetates into three different products. Factors such as negatively charged polyanion, positive valence band potential, intraband states, singlet oxygen sensitization, and multi-electron transfer contribute to this chromoselective conversion.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Review
Chemistry, Organic
Yevheniia Markushyna, Aleksandr Savateev
Summary: Photoredox catalysis has evolved into a mature field in chemistry, particularly in organic synthesis where sustainable alternatives to conventional methods are being developed. The selection of irradiation conditions, including mode, intensity, and wavelength, plays a crucial role in the outcome of photocatalytic reactions. By controlling these conditions, researchers can influence the reaction mechanism and access highly reactive species that are otherwise difficult to obtain.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Maria Jerigova, Yevheniia Markushyna, Ivo F. Teixeira, Bolortuya Badamdorj, Mark Isaacs, Daniel Cruz, Iver Lauermann, Miguel Angel Munoz-Marquez, Nadezda V. Tarakina, Nieves Lopez-Salas, Oleksandr Savateev, Pablo Jimenez-Calvo
Summary: By pre-organization of precursors and further co-polymerization, tunable semiconductors can be synthesized through anionic doping. These S-doped/C3N4-based materials demonstrate enhanced optical, electronic, structural, textural, and morphological properties, leading to higher performance in organic benzylamine photooxidation, oxygen evolution, and energy storage.
Article
Chemistry, Multidisciplinary
Yevheniia Markushyna, Markus Antonietti, Aleksandr Savateev
Summary: The use of visible light photocatalysis with a carbon nitride photocatalyst has enabled the synthesis of sulfonyl chlorides from arenediazonium salts with high yields. This method shows great versatility with different substrate electron properties and functional groups, providing a sustainable alternative to the Meerwein chlorosulfonylation reaction.
ACS ORGANIC & INORGANIC AU
(2022)
Article
Chemistry, Multidisciplinary
Christene A. Smith, Francesco Brandi, Majd Al-Naji, Ryan Guterman
Summary: Biorefinery utilizes a highly-active iridium complex as a low-temperature catalyst to produce precursors for epoxy resins from biomass waste streams, achieving the process at a lower temperature and providing a new avenue for biorefinery with lower energy demands.
Article
Chemistry, Multidisciplinary
Zhe She, Mina R. Narouz, Christene A. Smith, Amy MacLean, Hans-Peter Loock, Heinz-Bernhard Kraatz, Cathleen M. Crudden
CHEMICAL COMMUNICATIONS
(2020)