Article
Multidisciplinary Sciences
Evgeniy G. Gordeev, Kirill S. Erokhin, Andrey D. Kobelev, Julia Burykina, Pavel Novikov, Valentine P. Ananikov
Summary: Visible light photocatalysis is a promising chemical synthesis method, but the challenge lies in the need for dedicated reactors to achieve maximum efficiency. This study developed customized laboratory photoreactors with temperature stabilization and the ability to adapt different light sources. Two important reactor design concepts, multiple parallel experiments and scale-up synthesis, were explored. Practical evaluation showed that 3D printed reactors performed well in test reactions, demonstrating their utility.
SCIENTIFIC REPORTS
(2022)
Article
Chemistry, Multidisciplinary
Dongchun Zheng, Xiao-Li Zhao, Xueqi Yan, Weimin Xuan, Qi Zheng, Lianjun Wang, Wan Jiang
Summary: A family of transition-metal doped Ti-oxo clusters with diverse core structures have been successfully synthesized. Their photocurrent responses can be tuned by varying the heterometals, and the cobalt-doped cluster exhibits the highest H-2 evolution activity (32.5 mu mol g(-1) h(-1)) with good stability.
NEW JOURNAL OF CHEMISTRY
(2022)
Article
Chemistry, Organic
Zhen-Xiang He, Bo Yin, Xiao-Huan Li, Xian-Li Zhou, Hai-Ning Song, Jin-Bu Xu, Feng Gao
Summary: By using Eosin Y as a metal-free photocatalyst and O2 as an oxidant, this study introduces a new photochemical protocol for the efficient aerobic oxidation of benzyl alcohols to aldehydes or ketones under mild reaction conditions with high yields. The catalyst system exhibits good tolerance towards different functional groups and precise chemoselectivity, which can also be easily scaled-up to gram scale. Furthermore, the methodological applications in practical synthesis of various organic molecules and the primary reaction mechanism were examined.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Takashi Nakazono, Tohru Wada
Summary: The doubly N-confused hexaphyrin dinuclear cobalt complex (Co2DNCH) was shown to be an efficient water oxidation catalyst, outperforming the mononuclear cobalt porphyrin. Utilizing [Ru-II(bpy)(3)](2+) as a photosensitizer and S2O82- as a sacrificial electron acceptor, O-2 was produced with a high turnover number, turnover frequency, and quantum yield.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Physical
Olaf Morawski, Pawel Gawrys, Jaroslaw Sadlo, Andrzej L. Sobolewski
Summary: Under violet light irradiation, HATN catalyzes hydrogenation reactions in various alcohols, producing hydrogenated species. Experimental findings are consistent with theoretical predictions, demonstrating the impact of the excited state of the HATN-solvent molecular complex on hydrogen transfer reactions.
Article
Chemistry, Multidisciplinary
Tyler M. Brown, Hassan H. Fakih, Daniel Saliba, Jathavan Asohan, Hanadi F. Sleiman
Summary: A barrier for biological applications of DNA structures is their instability to nucleases. This study explores the use of UV-mediated thymine dimerization to crosslink and stabilize DNA nanostructures. The researchers compare different methods of DNA irradiation and show that all approaches can achieve nuclease protection, but with varying levels of off-target crosslinking and damage. They also demonstrate a mild irradiation condition that enhances serum stability while maintaining DNA function. This methodology has potential applications in nucleic acid therapy and nanotechnology.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Environmental Sciences
Yongwoo Kim, Jonghyun Kim, Michelle H. Wiebenga, Se H. Oh, Do Heui Kim
Summary: Currently, the automotive industry is transitioning from internal combustion engine vehicles to electric vehicles due to severe environmental issues. However, this transition will take more than 10 years, during which internal combustion engine vehicles are still necessary. The emissions from these vehicles, such as hydrocarbons and nitrogen oxides, contribute to environmental pollution. This study investigates the removal of hydrocarbons from the exhaust gas of gasoline and diesel engines using commercial Pd catalysts. The research examines the effects of Pd loading and aging process on the catalytic abilities and identifies the reaction pathway for the complete oxidation of propane. The findings also highlight the impact of different gas components in realistic exhaust gas on the catalyst's abatement abilities.
ENVIRONMENTAL POLLUTION
(2023)
Review
Chemistry, Multidisciplinary
Matthew J. Genzink, Jesse B. Kidd, Wesley B. Swords, Tehshik P. Yoon
Summary: Asymmetric photocatalysis is a major research topic in contemporary synthetic organic chemistry. However, the discovery of general strategies for highly enantioselective photochemical reactions has been a recent development, leading to a somewhat limited variety of stereocontrolled photoreactions. This review summarizes the chiral catalyst structures that have been studied for solution-phase asymmetric photochemistry, providing insight into the logic required for highly effective stereocontrolled photocatalysis.
Article
Chemistry, Physical
Ting Li, Yidan Liu, Rongrong Jia, Lei Huang
Summary: The article presents a novel approach to synthesize one-dimensional heterogeneous bimetallic nanochains using a local surface plasmon resonance (LSPR) based strategy. Through self-assembly and light stimulation, metal nanoparticles are connected to form chains. The obtained Au5Pt1 nanochains exhibit significantly improved catalytic performance in the electrocatalytic hydrogen evolution reaction.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2024)
Article
Chemistry, Multidisciplinary
Alexandra Walter, Wolfgang Eisenreich, Golo Storch
Summary: This study reports a photochemical approach using flavin catalysts to oxidize silyl enol ethers to α,β-unsaturated ketones. The catalysts exhibit good stability throughout the reaction and can be successfully applied in subsequent aerobic epoxidation reactions. The sequential catalytic activity of flavin enables rapid diversification of substrates.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Multidisciplinary Sciences
Virgil Andrei, Inwhan Roh, Peidong Yang
Summary: Artificial photosynthesis converts small molecules into useful fuels using photochemical diodes. Nanowire semiconductors offer advantages in light absorption and catalytic activity, but require careful integration for overall fuel production.
Article
Chemistry, Multidisciplinary
Changmin Hou, Zhao Cui, Sai Zhang, Wenlong Yang, Hongtao Gao, Xiliang Luo
Summary: Research has shown that a series of ultra-thin NiFe-LDH nanosheets prepared on a large scale via a rapid room-temperature method exhibit outstanding electrocatalytic performance towards water oxidation, due to the synergistic effect of more exposed active sites, efficient electron transport, and optimized OER kinetics.
Article
Nanoscience & Nanotechnology
B. Huang, X. C. Tang, C. Geng, Q. F. He, J. Yi, Q. Wang, W. X. Huang, Q. X. Yuan, Y. Yang, G. Wang, W. H. Wang
Summary: Using synchrotron X-ray nano-computed tomography and finite element analysis, we reconstructed the nanostructure of shear bands (SBs) and investigated their formation and evolution in a bent heterogeneous Pd-based metallic glass fiber. We found that in addition to plain SBs (PSBs), there were hidden SBs (HSBs) with density fluctuations inside the metallic glass. The HSBs had average densities 5%-25% smaller than the surrounding matrix and thicknesses ranging from 100 nm to 530 nm. The structures of the HSBs were closely related to the heterogeneous structure and local strain rate of the metallic glass.
MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING
(2023)
Article
Chemistry, Multidisciplinary
Cali Antolini, Charles D. Spellman Jr, Christopher J. Otolski, Gilles Doumy, Anne Marie March, Donald A. Walko, Cunming Liu, Xiaoyi Zhang, Benjamin T. Young, Joseph E. Goodwill, Dugan Hayes
Summary: This study investigates the formation and fate of Fe(V) and Fe(IV) species in aqueous potassium ferrate(VI) through a combination of optical and X-ray transient absorption spectroscopies. The results improve the mechanistic understanding and accelerate the development of novel advanced oxidation processes for water treatment applications.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Prangya P. Sahoo, Miroslav Mikolasek, Kristina Husekova, Edmund Dobrocka, Jan Soltys, Peter Ondrejka, Martin Kemeny, Ladislav Harmatha, Matej Micusik, Karol Frohlich
Summary: This study investigated the properties of metal-insulator-semiconductor (MIS) photoanodes with RuO2/SiO2/n-Si and IrO2-RuO2/SiO2/n-Si configurations for water oxidation. The results showed that both structures exhibited better oxygen evolution performance under acidic conditions compared to alkaline or near-neutral pH conditions.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Physical
Walid Dachraoui, Rolf Erni
Summary: This study utilizes in situ liquid cell scanning transmission electron microscopy to track the growth of Pd nanoparticles at the atomic scale. The results reveal that the formation of Pd nanoparticles involves multiple steps, including nonclassical nucleation and multi-step growth processes. These findings confirm the importance of element-specific interactions in determining the pathway of crystalline nanoparticle formation, even under identical synthesis conditions.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yuheng Jiang, Siyang Li, Shikun Wang, Yin Zhang, Chang Long, Jun Xie, Xiaoyu Fan, Wenshi Zhao, Peng Xu, Yingying Fan, Chunhua Cui, Zhiyong Tang
Summary: Selective and efficient CH4 oxidation to CH3OH and HCHO was achieved by precisely controlling the type of as-formed radicals through rational design on photocatalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Xiaobing Shi, Qianbao Wu, Chunhua Cui
Summary: This study reveals that quenching-treated WO3 with preferred (021) facets exhibits highly improved Faradaic efficiency and stability, while untreated WO3 generates abundant (OH)· radicals and suffers from performance degradation.
Article
Chemistry, Physical
Huifang Hu, Ying Kong, Menglong Liu, Viliam Kolivoska, Alexander V. Rudnev, Yuhui Hou, Rolf Erni, Soma Vesztergom, Peter Broekmann
Summary: The application of gas diffusion electrodes (GDEs) for the electrochemical reduction of CO2 to value-added products has the potential to achieve high current densities. However, maintaining stable operation at such high reaction rates is challenging due to the flooding of the GDE. The chemical composition of the applied catalyst inks, particularly the excessive presence of polymeric capping agents, can lead to the blockage of micropores and hinder effective electrolyte perspiration inside the GDE structure.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Nanoscience & Nanotechnology
Honglei Lu, Lei Li, Qianbao Wu, Shijia Mu, Ruijuan Zhao, Xia Zheng, Chang Long, Qing Li, Hongfei Liu, Chunhua Cui
Summary: Selective electrochemical upgrading of CO2 to multicarbon (C2+) products requires a C-C coupling process involving Cu oxidation states. This study reveals the critical role of Cu+ in promoting C-C coupling through coordination with a CO intermediate. Cu+ is dynamically stabilized by the presence of iodide (I-) in HCO3- electrolytes, leading to an increased C2+ Faradaic efficiency. Introducing CuI into I--containing HCO3- electrolytes enables a higher C2+ selectivity for direct CO electroreduction.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Nanoscience & Nanotechnology
Alexander Vogel, Alicia Ruiz Caridad, Johanna Nordlander, Martin F. Sarott, Quintin N. Meier, Rolf Erni, Nicola A. Spaldin, Morgan Trassin, Marta D. Rossell
Summary: Recent studies have found that oxygen defects on the surface of improper ferroelectric thin films can result in the loss of ferroelectric response. We investigated hexagonal YMnO3 thin films and discovered that the polarization suppression in thinner films is due to oxygen vacancies. We demonstrated that these vacancies form on the film surfaces to screen the large internal electric field. Furthermore, by modifying the oxygen concentration, we can significantly tune the phase transition temperatures. These findings are expected to be applicable to other ferroelectric oxide films, highlighting the importance of controlling oxygen content and cation oxidation states for successful integration in nanoscale applications.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Ivan Surin, Zhenchen Tang, Julian Geiger, Suyash Damir, Henrik Eliasson, Mikhail Agrachev, Frank Krumeich, Sharon Mitchell, Vita A. Kondratenko, Evgenii V. Kondratenko, Gunnar Jeschke, Rolf Erni, Nuria Lopez, Javier Perez-Ramirez
Summary: The discovery of low-valent manganese stabilized on ceria as a stable catalyst for ammonia oxidation to nitrous oxide offers a promising solution to the high manufacturing costs and suboptimal selectivity and stability of nitrous oxide synthesis. The catalyst exhibits higher productivity than state-of-the-art alternatives and establishes a structure-performance relationship.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Physical
Jiawei Du, Shuaihu Jiang, Ruya Zhang, Pai Wang, Chao Ma, Ruijuan Zhao, Chunhua Cui, Yanning Zhang, Yijin Kang
Summary: Electrochemical production of H2O2 via 2e- ORR using Pd with Cu electrodeposition as model material shows promising potential in terms of safety, efficiency, and decentralization. The introduction of Cu promotes the production of H2O2 by stabilizing Pd-O and improving 2e- ORR activity according to spectroscopic analysis and computation. PdCu nanowire synthesis demonstrates high selectivity and production rate towards H2O2.
Article
Chemistry, Multidisciplinary
Thaylan Pinheiro Araujo, Jordi Morales-Vidal, Georgios Giannakakis, Cecilia Mondelli, Henrik Eliasson, Rolf Erni, Joseph A. Stewart, Sharon Mitchell, Nuria Lopez, Javier Perez-Ramirez
Summary: Ternary Pd-In2O3/ZrO2 catalysts prepared by wet impregnation exhibit selective and stable architecture under CO2 hydrogenation conditions, irrespective of the order of addition of Pd and In phases on the zirconia carrier. The rapid restructuring of the catalysts is driven by the metal-metal oxide interaction energetics. The presence of InPdx alloy particles decorated by InOx layers prevents performance losses associated with Pd sintering.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Multidisciplinary Sciences
Mengjun Xiao, Qianbao Wu, Ruiqi Ku, Liujiang Zhou, Chang Long, Junwu Liang, Andraz Mavric, Lei Li, Jing Zhu, Matjaz Valant, Jiong Li, Zhenhua Zeng, Chunhua Cui
Summary: In this study, an amorphous CoOxCly catalyst was deposited in situ in an acidic saline electrolyte containing Co2+ and Cl- ions to enhance the selectivity and stability of chlorine evolution in the chlor-alkali industry. In situ spectroscopic studies and theoretical calculations revealed that Cl- acted as a promoter to enhance the chlorine evolution by preventing the higher oxidation state of Co sites, thus suppressing the oxygen evolution reaction.
NATURE COMMUNICATIONS
(2023)
Article
Materials Science, Multidisciplinary
Alexander Vogel, Alicia Ruiz-Caridad, Johanna Nordlander, Rolf Erni, Morgan Trassin, Marta D. Rossell
Summary: In this study, the crystal and electronic structure of YMnO3 thin films were investigated using scanning transmission electron microscopy and electron energy loss spectroscopy. The phase transition and changes in the electronic structure were observed and analyzed. The study demonstrated the sensitivity of the O-K near-edge structure to structural distortions in YMnO3 polymorphs, providing important insights for future research on polymorphic phase transformations in improper ferroelectrics.
Article
Chemistry, Multidisciplinary
Yuheng Jiang, Siyang Li, Shikun Wang, Yin Zhang, Chang Long, Jun Xie, Xiaoyu Fan, Wenshi Zhao, Peng Xu, Yingying Fan, Chunhua Cui, Zhiyong Tang
Summary: We have achieved high selectivity and high productivity of CH3OH and HCHO in CH4 photooxidation for the first time by precisely controlling the type of as-formed radicals through rational design on photocatalysts. By tuning the band structure and active sites (single atoms or nanoparticles) on Au/In2O3 catalysts, we can generate two different radicals, center dot OOH and center dot OH, leading to the formation of CH3OH and HCHO, respectively. The results show remarkable selectivity and yield of HCHO (97.62% and 6.09 mmol g(-1)) on In2O3-supported Au single atoms (Au-1/In2O3) and exceptional selectivity and yield of CH3OH (89.42% and 5.95 mmol g(-1)) on In2O3-supported Au nanoparticles (AuNPs/In2O3) during photocatalytic CH4 oxidation at room temperature for 3 hours. This work opens up a new avenue for efficient and selective CH4 oxidation through the design of composite photocatalysts.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Xianwei Wang, Jiangtao Zhao, Henrik Eliasson, Rolf Erni, Abolfazl Ziarati, Siobhan Mckeown Walker, Thomas Burgi
Summary: Depositing Au-25 nanoclusters onto a manganese oxide support produces a stable and highly active catalyst. By optimizing the pretreatment temperature, the performance of the Au-25/MnO2 catalyst in low-temperature CO oxidation can be significantly enhanced.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Nanoscience & Nanotechnology
Chiara Ricca, Elizabeth Skoropata, Marta D. Rossell, Rolf Erni, Urs Staub, Ulrich Aschauer
Summary: A highly ordered Moire dislocation lattice has been discovered recently, and the structure and defect chemistry of these dislocations have been investigated through experimental characterization and computational calculations. The results show the presence of undercoordinated light metal cations and oxygen vacancies at the dislocation cores, which may affect the properties of complex multifunctional heterostructures and result in the reduction of Ti ions through electron doping.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Henrik Eliasson, Yubiao Niu, Richard E. Palmer, Henrik Gronbeck, Rolf Erni
Summary: Based on scanning transmission electron microscopy, direct evidence is provided to show how the metal-support interaction affects the structure of supported nanoparticles. It is found that Pt nanoparticles on CeO2 exhibit facet-dependent support interaction, which determines the dimensionality of the particles. Pt particles consisting of less than approximately 130 atoms prefer a 3D shape on CeO2(111) facets, while 2D raft structures are favored on CeO2(100) facets.