Article
Chemistry, Applied
Lilian Geniller, Marc Taillefer, Florian Jaroschik, Alexis Prieto
Summary: The Ni-photoredox catalyzed desulfurative cross-coupling reaction enables the synthesis of various unsymmetrical diarylmethane molecules under mild reaction conditions, providing new transformations of abundant, naturally occurring thiols.
ADVANCED SYNTHESIS & CATALYSIS
(2022)
Article
Chemistry, Physical
Danae A. Chipoco Haro, Eri Muramoto, Robert J. Madix, Juan Carlos F. Rodriguez-Reyes
Summary: Alkynes are nucleophiles that can easily undergo dehydrogenation on a gold catalyst, forming acetylide species and coupling products. However, the strong attachment of catalytic intermediates to the surface can lead to parallel decomposition pathways and carbon poisoning of the catalyst. Alkynes can displace species known for facile dehydrogenation on gold, including adsorbed alkoxy and alcohols of similar molecular weight.
Article
Chemistry, Physical
Mohammad S. AlQahtani, Xiaoxing Wang, Sean D. Knecht, Sven G. Bilen, Chunshan Song
Summary: A thorough evaluation of surface reactions under plasma conditions was conducted, revealing a new Eley-Rideal reaction between plasma-generated atomic hydrogen and strongly adsorbed SO2 over alumina; plasma induced partial desorption of SO2 species, enhanced strong chemisorption of SO2 over supported iron sulfide catalyst, and facilitated H-2 chemisorption and reaction with iron sulfide, resulting in sulfur vacancies.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Organic
Qi Zhu, En Zhao, Yajing Shen, Zupeng Chen, Weiwei Fang
Summary: An easy to prepare nickel-coordinated mesoporous graphitic carbon nitride (Ni-mpg-CN) was used as a heterogeneous photocatalyst to efficiently catalyze the photocatalytic C-N cross-coupling of (hetero)aryl bromides and aliphatic amines, yielding the desired monoaminated products in good yields. Furthermore, the synthesis of the pharmaceutical tetracaine was successfully achieved, highlighting its practical applicability.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2023)
Article
Chemistry, Organic
Shuai Zhong, Zhiwei Zhou, Feng Zhao, Guojiang Mao, Guo-Jun Deng, Huawen Huang
Summary: In this study, sulfinates were successfully used as sulfenylating reagents in C-S couplings through visible-light-induced photo/nickel dual catalysis under base- and external reductant-free conditions. The method showed high selectivity and tolerance towards various functionalities.
Article
Chemistry, Multidisciplinary
Cui-Cui Li, Siqi Zhang, Jian Tang, Ruijun Jian, Yu Xia, Liang Zhao
Summary: This study develops a two-step synthetic method to achieve three unprecedented aryl dicarbanion-bonded Ag-13 nanoclusters using protective macrocyclic ligands. The research not only reveals the formation and evolution process of cluster species in catalytic reactions but also discovers novel inter- and intra-cluster coupling steps.
Article
Chemistry, Physical
Lin-Yan Bao, Rong-Wan Gao, Shuang Wang, Run-Han Li, Bo Zhu, Zhong-Min Su, Wei Guan
Summary: Photoredox/transition-metal dual catalysis is an efficient method for constructing C-N bonds. However, low recovery, low utilization rate, and high cost have hindered its application and development. By utilizing zinc powder, the oxidation state of nickel was successfully regulated, achieving a catalytic cycle without light.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Yuting Li, Yu Tang, Franklin (Feng) Tao
Summary: This article reports a new supported catalyst, Rh-1/P25, consisting of singly dispersed Rh-1 atoms anchored on TiO2 (P25) nanoparticles. The Rh-1/P25 catalyst exhibits high activity for C-N coupling and demonstrates selectivity of higher than 90% for producing tertiary amines in six hydroaminoalkylation reactions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Applied
Mingyang Gao, Jiamin Wang, Weixiang Shang, Yuchao Chai, Weili Dai, Guangjun Wu, Naijia Guan, Landong Li
Summary: Suzuki-Miyaura cross-coupling reaction is a powerful method to construct carbon-carbon bonds and is widely used in the synthesis of functional organic compounds. In this study, zeolite-encased Pd particles (Pd@MFI) were successfully prepared and investigated as promising heterogeneous catalysts for the Suzuki-Miyaura cross-coupling reaction. The Pd@MFI catalysts showed high activity, with dispersed Pd particles efficiently stabilized within the MFI zeolite matrix. The presence of basic sites adjacent to Pd sites was crucial for achieving high catalytic activity.
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.
Article
Chemistry, Multidisciplinary
Zhijun Li, Xiaowen Lu, Rufang Zhao, Siqi Ji, Mingyang Zhang, J. Hugh Horton, Yang Wang, Qian Xu, Junfa Zhu
Summary: Researchers have developed an efficient molten-salt-assisted approach to create atomically dispersed cobalt atoms supported over vanadium pentoxide layered material. This cobalt single-atom catalyst achieves extraordinary catalytic efficiency in the dehydrogenative coupling reaction of alcohols and amines, with high selectivity and conversion. Density functional theory calculations confirm the optimized coordination environment and strong metal-support interaction contribute significantly to the activation of reactants.
Review
Chemistry, Physical
Ubong J. Etim, Peng Bai, Oz M. Gazit, Ziyi Zhong
Summary: This article discusses the importance of oxidation reactions in the origin of life and industrial applications. The development of green catalysis enables catalytic reactions to be conducted at mild conditions. Activating oxygen molecules under mild conditions remains a major challenge in catalytic oxidation reactions.
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING
(2023)
Article
Nanoscience & Nanotechnology
Xuewen Guo, Jabor Rabeah, Ruixue Sun, Dengxu Wang, Esteban Mejia
Summary: A series of hybrid porous polymers (HPPs) based on polyhedral oligomeric silsesquioxane (POSS) were synthesized and successfully used as metal-free heterogeneous photocatalysts for cross-dehydrogenative coupling reactions, showing efficient catalytic performance under visible light. The novel catalysts can be easily recovered and reused, with mechanistic investigations revealing the oxidation-reduction process during photoexcitation.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Organic
Ge Liang, Jing-Hao Wang, Tao Lei, Yuan-Yuan Cheng, Chao Zhou, Ya-Jing Chen, Chen Ye, Bin Chen, Chen-Ho Tung, Li-Zhu Wu
Summary: This study presents an aerobic metal-free, visible-light-induced regioselective thiolation of phenols with thiophenols, showing high functional group tolerance and selectivity. Mechanistic studies reveal the crucial role of disulfide radical cation in the visible-light catalysis of aerobic thiolation, allowing selective formation of sulfide or sulfoxide products with high activity in a one-pot reaction by controlling the equivalent ratio of substrates.
Article
Chemistry, Physical
Lukas Hoff, Gleb A. Chesnokov, Anthony Linden, Karl Gademann
Summary: This study presents a thorough mechanistic investigation of the Pd-catalyzed and Ag-mediated cross-coupling reaction between monosubstituted tetrazine and boronic acids. Through kinetic analyses, isolation of intermediates, and computational methods, insights into the mechanism were obtained. The study also demonstrated the experimental confirmation of a highly electron-deficient ligand and the impact of mechanistic understanding on the generality of the reaction scope through a data-driven workflow.
Article
Gastroenterology & Hepatology
Erica M. Valdovinos, Bradley W. Frazee, Christian Hailozian, Daniel A. Haro, Andrew A. Herring
JOURNAL OF CLINICAL GASTROENTEROLOGY
(2020)
Article
Chemistry, Multidisciplinary
Miguel Gakiya-Teruya, Luis Palomino-Marcelo, Scott Pierce, Alfredo M. Angeles-Boza, Vijay Krishna, Juan Carlos F. Rodriguez-Reyes
JOURNAL OF NANOPARTICLE RESEARCH
(2020)
Article
Engineering, Chemical
Renzo E. Portilla, Chuan He, Melissa Jacome-Collazos, Karinna Visurraga, Humberto Chirif, Andrew Teplyakov, Juan Carlos F. Rodriguez-Reyes
MINERALS ENGINEERING
(2020)
Article
Chemistry, Physical
Danae A. Chipoco Haro, Eri Muramoto, Robert J. Madix, Juan Carlos F. Rodriguez-Reyes
Summary: Alkynes are nucleophiles that can easily undergo dehydrogenation on a gold catalyst, forming acetylide species and coupling products. However, the strong attachment of catalytic intermediates to the surface can lead to parallel decomposition pathways and carbon poisoning of the catalyst. Alkynes can displace species known for facile dehydrogenation on gold, including adsorbed alkoxy and alcohols of similar molecular weight.
Article
Engineering, Chemical
Gonzalo Larrabure, Juan Carlos F. Rodriguez-Reyes
Summary: The ongoing depletion of gold and silver-containing ore deposits requires a shift towards processing more complex sources. Challenges in extracting gold or silver from refractory sources include kinetic or thermodynamic impediments, preg-robbing effects, and excessive cyanide consumption. Strategies to overcome these challenges include intensive grinding, oxidation processes, surface destruction, and the addition of competitors for preg-robbing.
MINERALS ENGINEERING
(2021)
Article
Archaeology
Angelica Isa-Adaniya, Anibal Alviz-Meza, Juan Carlos F. Rodriguez-Reyes
Summary: Funding for culture and heritage projects is usually limited, and even more so during times of crisis. The Research Center for Heritage Conservation in Lima, Peru, has adopted the value-chain model to evaluate conservation projects and promote sustainable practices. Projects must meet the criteria of well-documented problem, clear hypothesis or objective, realistic methodology, and practical and beneficial results. The application of the value-chain model leads to tangible outcomes and facilitates self-sustaining conservation research.
STUDIES IN CONSERVATION
(2022)
Article
Chemistry, Multidisciplinary
Luis Palomino, Danae A. Chipoco Haro, Miguel Gakiya-Teruya, Feng Zhou, Adolfo La Rosa-Toro, Vijay Krishna, Juan Carlos F. Rodriguez-Reyes
Summary: Novel silver nanoparticles were synthesized using polyhydroxy fullerene as a reducing and capping agent, showing smaller size, enhanced antibacterial activity, and improved electrocatalytic properties compared to conventional citrate-synthesized nanoparticles.
Article
Chemistry, Physical
Danae A. Chipoco Haro, Layla M. Gonzales Matushita, Maynard J. Kong, Juan Carlos F. Rodriguez-Reyes
Summary: This study compares the interaction of aromatic compounds with gold surfaces and finds that the introduction of functional groups significantly increases the adsorption energy, affecting the pathways for decomposition and poisoning reactions. Furthermore, the molecular structure of the aromatic molecule determines the extent to which further dehydrogenation, coupling, or surface decomposition reactions occur.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Archaeology
A. Alviz-Meza, D. A. Chipoco Haro, J. Tello-Hijar, M. I. Velarde, C. Benndorf, J. C. Rodriguez-Reyes, S. Ismat Shah
Summary: Between 150 BCE and 700 CE, Peruvian goldsmiths in the northern coastline developed two electrochemical gilding methods for copper. The first method involved immersing the copper in a gold-containing solution, while the second method utilized the same solution with the addition of pyrite to form a galvanic cell. XRF and SEM-EDX characterizations showed that the second method resulted in a more homogeneous deposition of gold with thicknesses similar to archaeological samples. This research contributes to our understanding of pre-Columbian techniques lost before the Inca Empire.
JOURNAL OF ARCHAEOLOGICAL SCIENCE-REPORTS
(2023)
Review
Chemistry, Multidisciplinary
Hakhyeon Song, Danae A. Chipoco Haro, Po-Wei Huang, Luisa Barrera, Marta C. Hatzell
Summary: In this article, recent advances and challenges in achieving sustainable urea synthesis are discussed. The current method for urea production, the Bosch-Meiser process, relies heavily on fossil fuels and leaves a significant carbon footprint. Shifting towards photochemical or electrochemical processes shows promise for complete electrification of urea synthesis, but there are challenges related to catalyst design, electrolyte optimization, and reactor engineering. The adoption of renewable energy sources is also crucial for the environmental impact of urea production.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Chemistry, Physical
Erhao Gao, Wenjing Feng, Qi Jin, Li Han, Yi He
Summary: The influence of K-doping on the reactive oxygen species and elementary reactions of HCHO catalytic oxidation was investigated using density functional theory (DFT). The introduction of K-doping changed the electronic structures of Ce and O, facilitating the adsorption and activation of HCHO and O2 molecules, enhancing lattice oxygen mobility, and reducing the energy barrier for HCHO oxidation. K-doping also promoted the formation of hydroxyl groups, facilitating HCHO adsorption and oxidation.
Article
Chemistry, Physical
Hao Fu, Zhangliang Xu
Summary: In this study, the adsorption mechanisms and detection performance of formaldehyde, ammonia, and sulfur dioxide on undoped and metal-doped ZnO surfaces were investigated using density functional theory. The results showed that formaldehyde and ammonia were physically adsorbed on the undoped ZnO surface, while sulfur dioxide was weakly chemisorbed. The adsorption energy was enhanced when ZnO was doped with metals. These findings provide theoretical guidance for the application of ZnO substrate materials in gas sensitivity research.
Article
Chemistry, Physical
Atsushi Nomura, Tohru Kurosawa, Migaku Oda, Satoshi Demura, Shogo Kuwahara, Sora Kobayashi, Hideaki Sakata
Summary: The study investigates the tunneling spectra of 1T-TiSe2 in the CDW state and the dip structure below the Fermi level, aiming to determine whether this dip is a CDW gap. The answer to this question is crucial for understanding the driving mechanism of CDW.
Article
Chemistry, Physical
A. S. Petrov, D. I. Rogilo, A. I. Vergules, V. G. Mansurov, D. V. Sheglov, A. V. Latyshev
Summary: This study investigates Si mass transport and morphological transformations on the Si(111) surface during (root 3 x root 3)-Sn reconstruction formation and Si homoepitaxy. The research shows that the formation of different Sn phases at different temperatures affects the Si island nucleation and monatomic step shift, which in turn impact the morphology of the Sn/Si(111) interface. Electromigration-induced drift of disordered Sn domains leads to enhanced noncompensated Si mass transport and surface roughening.
Article
Chemistry, Physical
D. V. Gruznev, L. V. Bondarenko, A. Y. Tupchaya, A. A. Yakovlev, A. N. Mihalyuk, A. V. Zotov, A. A. Saranin
Summary: Deposition of thallium (Tl) onto the Au/Si(111)5 x 2 reconstruction followed by annealing results in the formation of a surface structure with 4 x 2 periodicity. The immiscibility of Au and Tl leads to the migration of Tl atoms over the Si chains. Thallium donates electrons to the surface, converting the metallic surface into an insulating state and altering the inter-chain distance within the array of Au atomic wires.
Article
Chemistry, Physical
Simone Giusepponi, Francesco Buonocore, Barbara Ferrucci, Massimo Celino
Summary: Using ab-initio calculations, the interaction between lead adatom and both clean and doped iron (100) surfaces was investigated. It was found that the lead adatom prefers to adsorb in the hollow site, which is more stable compared to the top and bridge sites, and in this position, it is energetically favorable over the iron adatom. Moreover, lead adsorbed in the hollow site of the iron (100) surface doped with chromium was found to create a more stable system compared to nickel-doped surfaces with an iron adatom in the same position. The study also explored inter-layer distances, bonding mechanisms, magnetic behaviors, and charge density differences. The results provide insights into the role of doping in the interaction between lead adatom and iron surface, and have implications for the analysis of corrosion processes caused by liquid lead.
Article
Chemistry, Physical
Shuo Zhang, Jin-Ho Choi
Summary: The recent synthesis of two-dimensional layered WSi2N4 has attracted attention due to its potential applications. This study investigates the catalytic performance of WSi2N4 monolayers with nitrogen vacancies in the hydrogen evolution reaction using first-principles calculations. The results show that the defective WSi2N4 monolayers exhibit remarkably high catalytic activity comparable to platinum catalysts. Electronic structure calculations also reveal the emergence of spin-polarized states due to the introduction of nitrogen vacancies.
Article
Chemistry, Physical
Xiaoyan Yu, Xin Cao, Wei Kang, Shanhua Chen, Ao Jiang, Yuhao Luo, Wenwei Deng
Summary: First-principles calculations were used to investigate the electronic properties of a TiO2 heterostructure modified with Bi2Te3 co-catalyst. The study revealed that the Bi2Te3/TiO2 interface introduced optimal band offsets, effectively suppressing electron-hole recombination and enhancing the utilization efficiency of photo-generated carriers. Additionally, the Bi2Te3 co-catalyst introduced extra catalytic active sites, further boosting the photo-catalytic hydrogen evolution efficiency.
Article
Chemistry, Physical
Filippo Longo, Emanuel Billeter, Selim Kazaz, Alessia Cesarini, Marin Nikolic, Aarati Chacko, Patrik Schmutz, Zbynek Novotny, Andreas Borgschulte
Summary: Alkaline water electrolysis is a simple and efficient method for renewable hydrogen production, utilizing cheap and abundant transition metals. The catalytic properties of Ni materials are enhanced by the formation of oxidized compounds on the surface. The high electrocatalytic activity of Ni (oxy)-hydroxides is directly related to water intercalation in the passivation layer, supporting the hypothesis of a water mediated OH- diffusion mechanism. The self-organization of the surface structure during passivation layer formation enables high electrode performance.
Article
Chemistry, Physical
Mohan Kumar Kuntumalla, Miriam Fischer, Alon Hoffman
Summary: By investigating the bonding, retention, and thermal stability of nitrogen in H-Diamond (100), it was found that nitrogen can partially recover its bonding with carbon atoms after high-temperature annealing, indicating a high thermal stability of nitrogen in diamond.
Article
Chemistry, Physical
Dong Yue, Liangying Wen, Rong Chen, Jianxin Wang, Zhongqing Yang
Summary: The adsorption behavior of Cl2 molecules on the TiC surface and the formation and transfer of reaction products were studied using first-principles ab initio calculations. The results show that the Cl atoms bonded to the surface Ti atoms are more stable, and the TiCl3 intermediate is easier to form than the TiCl2 intermediate.
Article
Chemistry, Physical
Yatao Wang, Peng Zhang, Hongjuan Li, Qiuju Xu, Shujun Liu, Xiaopeng Liu, Xuehua Guo, Yitao Li, Jinzhang Liu, Sen Dong, Zhi Wei Seh, Qianfan Zhang
Summary: In this study, the adsorption performance of two types of metal-organic frameworks (MOFs) for thiophene and benzene was experimentally investigated. The results showed that IZE-1 exhibited high selectivity and superior adsorption capacity for thiophene, especially at low concentrations. First-principles calculations and molecular dynamics simulations provided insights into the mechanism of thiophene adsorption and the high selectivity observed. This research demonstrates the potential of MOFs for thiophene adsorption, particularly at high concentrations.
