Article
Environmental Sciences
Guy Didier Fanou, Mamadou Traore, Benjamin Kouassi Yao, Andrei Kanaev, Khay Chhor
Summary: A new composite photocatalyst was developed by grafting size-selected 5-nm titanium-oxo-alkoxo nanoparticles onto P25-TiO2 nanoparticles and incorporating HAP obtained by co-precipitation of salts. The photocatalytic yield was increased for the composite photocatalysts with the addition of HAP, likely due to a synergy between adsorption and photo-oxidation.
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
(2021)
Article
Chemistry, Applied
Haihang Tong, Dezhi Shi, Huayi Cai, Jiayu Liu, Mengying Lv, Li Gu, Ling Luo, Bin Wang
Summary: Novel hydrothermal methods assisted by hydroxyapatite were used to solidify heavy metals in fly ash, resulting in hydrothermally-treated products that meet landfilling standards. The solidification mechanism involved the formation of stable compounds between hydroxyapatite and heavy metal ions. The addition of hydroxyapatite seed crystal improved the solidification efficiency.
FUEL PROCESSING TECHNOLOGY
(2022)
Article
Multidisciplinary Sciences
Haigen Fu, Jingzhe Cao, Tianzhang Qiao, Yuyin Qi, Simon J. Charnock, Samuel Garfinkle, Todd K. Hyster
Summary: This study reports a highly chemoselective and enantioselective Csp(3)-Csp(3) XEC reaction catalyzed by flavin-dependent 'ene'-reductases (EREDs). The photoexcitation of the enzyme-templated charge-transfer complex enables the chemoselective reduction of alkyl halides and high enantioselectivity.
Article
Chemistry, Organic
Vinita Yadav, Sayali G. Jagtap, Ekambaram Balaraman, Santosh B. Mhaske
Summary: A novel method for the synthesis of N-substituted indoles under additive and base-free conditions is reported. The method utilizes a one-pot cascade approach with water as the only stoichiometric byproduct. The catalytic system used in this transformation exhibits high efficiency. A diverse range of N-alkylated indoles can be synthesized using various substrates.
Article
Multidisciplinary Sciences
Xiaomin Shu, De Zhong, Qian Huang, Leitao Huan, Haohua Huo
Summary: Site- and enantioselective alpha-acylation of saturated N-heterocycles with in situ-activated carboxylic acids is achieved using a modular approach that combines hydrogen-atom-transfer reactivity of photocatalytically generated chlorine radicals with asymmetric nickel catalysis. This strategy selectively functionalizes cyclic alpha-amino C-H bonds without affecting benzylic, allylic, acyclic alpha-amino, and alpha-oxy methylene groups. The protocol displays excellent chemo-, site-, and enantioselectivity and can be used for late-stage diversification, including the synthesis of previously inaccessible Taxol derivatives.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Applied
Maoling Tao, Lin-Yuan Zeng, Weipiao Li, Guoliang Pu, Jia Jia, Qiuli Yao, Xuefei Li, Chun-Yang He
Summary: We have developed a decarboxylative coupling reaction between N-hydroxyphthalimide esters and bromopolyfluorobenzene, which is facilitated by the synergetic action of Hantzsch ester, photoredox catalyst, and nickel catalyst. This method allows for the efficient conversion of primary and secondary alkyl carboxylic acids into polyfluoroaryl compounds, demonstrating broad scope and excellent functional group compatibility. Furthermore, we have successfully demonstrated the applicability of this method in the direct modification of amino acids and biologically active molecules.
ADVANCED SYNTHESIS & CATALYSIS
(2023)
Article
Chemistry, Multidisciplinary
Yanmei Guo, Yongbing Lou, Jinxi Chen, Yixin Zhao
Summary: Lead-free double perovskite nanocrystals show high efficiency in photocatalysis, with improved performance achieved through rational control of surface ligands. The results indicate significant potential for organic synthesis and chemical transformations.
Article
Chemistry, Organic
Sheng-Yun Zhou, Ding Zhang, Xiao-Jie Liu, Jing-Hao Qin, Zheng-Li Fu, Shuang-Long Li, Fang-Jun Cai, Yang Li, Jin-Heng Li
Summary: A novel photoredox-catalyzed C(sp(3))-C(sp(3)) cross-coupling reaction between N-arylamines and cycloketone oxime esters has been achieved under mild conditions. The redox-neutral reaction shows good functional group tolerance and excellent regioselectivity without the need for additional base or ligand control. Furthermore, this approach has been successfully applied for the late-stage modification of short peptides and analogues.
ORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Biochemistry & Molecular Biology
Guozhen Wang, Tong Lu, Xinjiang Zhang, Mengna Feng, Chengshuang Wang, Wei Yao, Shunchao Zhou, Zhenzhou Zhu, Wenping Ding, Meng He
Summary: The introduction of HAP nanoparticles effectively improved the properties of cellulose hydrogel, enhancing thermal stability, compressive strength, and adsorption capacity towards Cu2+. The study shows wide potential applications of the cellulose/HAP nanocomposite hydrogels.
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
(2021)
Article
Materials Science, Ceramics
S. V. Rempel, D. A. Eselevich, H. Schroettner, A. A. Valeeva, A. A. Rempel
Summary: The study investigated the structural and thermal behavior of TiOy/HAp nanocomposite materials used in tissue engineering through various analysis methods. It was found that the TiOy additives have a stabilizing effect on HAp composites, with different stoichiometries impacting the interactions between the matrix and nanoparticles.
CERAMICS INTERNATIONAL
(2021)
Article
Chemistry, Organic
Yang -yang Li, Bing Gao
Summary: N-functionalization of free sulfoximines is a significant method for modifying their properties for various applications. This study presents a rhodium-catalyzed N-allylation of free sulfoximines (=NH) with allenes, enabling chemo- and enantioselective ?-hydroamination of allenes and gem-difluoroallenes. The synthesis of sulfoximine products using this method is also demonstrated.
Article
Chemistry, Physical
Raluca-Stefania Danila, Ioan Dumitru, Maria Ignat, Aurel Pui
Summary: A CoFe2O4@HaP nanocomposite was synthesized and used for the adsorption of Congo Red dye from aqueous solutions. Characterization techniques confirmed the structure and properties of the nanocomposite. The nanocomposite exhibited high adsorption capacity and good fitting to a pseudo-second-order kinetic model.
Article
Materials Science, Multidisciplinary
Chenning Zhang, Tetsuo Uchikoshi, Lihong Liu, Kaori Iwanami-Kadowaki, Masayoshi Uezono, Keiji Moriyama, Masanori Kikuchi
Summary: Antibacterial-functionalized Ag-loaded hydroxyapatite coatings were successfully fabricated by the EPD process, showing potential application in implant surgery for preventing bacterial infection. The coatings have strong adhesion due to the use of Mg2+ as an inorganic binder. This surface antibacterial function improves surgical success.
Article
Chemistry, Organic
Huiping Yin, Tianjiao Huang, Bai Shi, Wei Cao, Chenxia Yu, Tuanjie Li, Kai Zhang, Changsheng Yao
Summary: A practical, convenient, and facile method for constructing highly functionalized 2-pyrrolidinone has been developed using N-heterocyclic carbene (NHC)-catalyzed radical tandem cyclization (30 examples, up to 94% yield). The method is transition metal-free and exhibits broad substrate scope, excellent functional group compatibility, and high efficiency.
ORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Organic
Akash Jana, Sayandip Chakraborty, Koushik Sarkar, Biplab Maji
Summary: In this study, we report the ruthenium-catalyzed synthesis of fi-alkylated secondary alcohols through the regioselective ring opening of epoxides with primary alcohols. The reaction employs alcohol as the carbon source and terminal reductant, and operates through tandem Markovnikov selective transfer hydrogenation of terminal epoxides and hydrogen transfer-mediated cross-coupling of the resulting alcohol with primary alcohol substrates. A broad scope of substrates, including drug and natural product derivatives, is demonstrated with excellent regioselectivity.
JOURNAL OF ORGANIC CHEMISTRY
(2023)
Review
Chemistry, Multidisciplinary
Justin C. Bui, Chanyeon Kim, Alex J. King, Oyinkansola Romiluyi, Ahmet Kusoglu, Adam Z. Weber, Alexis T. Bell
Summary: The electrochemical reduction of carbon dioxide (CO2R) driven by renewable electricity offers a promising route for reusing CO2 and producing carbon-containing chemicals and fuels sustainably. Optimizing the catalyst microenvironment and selectivity, as well as controlling the electrolyte and operating conditions, are crucial for achieving economic viability and high product yields.
ACCOUNTS OF CHEMICAL RESEARCH
(2022)
Correction
Energy & Fuels
Chanyeon Kim, Justin C. Bui, Xiaoyan Luo, Jason K. Cooper, Ahmet Kusoglu, Adam Z. Weber, Alexis T. Bell
Review
Chemistry, Multidisciplinary
Justin C. Bui, Eric W. Lees, Lalit M. Pant, Iryna V. Zenyuk, Alexis T. Bell, Adam Z. Weber
Summary: Electrochemical synthesis using renewable energy to convert feedstocks into chemicals and fuels is promising, but understanding phenomena in porous electrode systems is challenging. Continuum modeling aids in understanding observed behaviors and guiding next-generation device design. Simulating multiscale phenomena in porous electrodes helps understand and improve the performance of electrochemical synthesis devices.
Article
Multidisciplinary Sciences
Hassan A. Aljama, Martin Head-Gordon, Alexis T. Bell
Summary: In this study, a high-throughput screening process using density functional theory was implemented to identify the energetically most favorable active sites in cation exchanged-zeolites, which is important for understanding catalysis and adsorption behaviors in zeolites.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Joseph A. Gauthier, Zhou Lin, Martin Head-Gordon, Alexis T. Bell
Summary: This study investigates the mechanism of CO2RR under experimental conditions and reveals the differences in activation barriers between alkaline and acidic pathways, as well as the kinetic favorability of COH formation under high overpotential.
ACS ENERGY LETTERS
(2022)
Article
Chemistry, Physical
Tianyu Zhang, Justin C. Bui, Zhengyuan Li, Alexis T. Bell, Adam Z. Weber, Jingjie Wu
Summary: In this study, we developed segmented gas-diffusion electrodes (s-GDEs) to improve the management of CO intermediates in tandem catalysts, thereby enhancing C2+ Faradaic efficiency and current density.
Article
Chemistry, Physical
Paul Kim, Jeroen Van der Mynsbrugge, Martin Head-Gordon, Alexis T. Bell
Summary: Passive NOx adsorbers (PNAs) are proposed for trapping NOx in automotive exhaust during cold start. In this study, it is found that Pd+ cations can be formed through water adsorbed on zeolite acid sites and can be fully desorbed by adsorbing NO. These reactions are thermodynamically feasible and Pd+ is not formed in the absence of adsorbed water and can be readily reoxidized to Pd2+ by trace amounts of O2.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Engineering, Chemical
Can Ekici, Christopher R. Ho, Joseph F. DeWilde, Lorenz T. Biegler, Paul M. Witt
Summary: This study presents the development and application of optimization strategies for mixed-catalyst, single-shot reactors in syngas to olefin (STO) processes. Finding the optimal catalyst distribution is challenging due to poorly conditioned singular optimal control problems. The graded bed and partial-moving finite-element approaches were used to maximize the olefins yield. An increase of 1.3% in yield was achieved from one zone to three zones, and further improved by 0.2% to the infinite dimensional solution. These improvements can be implemented without additional investment. The results suggest the potential application of mixed-catalyst single shot reactor beds for enhancing reactor performance in other reaction mechanisms.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Liang Qi, Sonali Das, Yanfei Zhang, Danna Nozik, Bruce C. Gates, Alexis T. Bell
Summary: Catalysts for ethene hydroformylation were prepared by grafting Rh into nests of -SiOZn-OH or -SiOCo-OH species in BEA zeolite. The Rh dispersion increased with increasing M/Rh ratio and had a positive effect on the turnover frequency for ethene hydroformylation. The Co-containing catalyst exhibited higher activity and selectivity than the Zn-containing catalyst.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Danna Nozik, Alexis T. Bell
Summary: Ethane and propane derived from shale gas are preferred feedstocks for the production of aromatics. Ga/H-MFI zeolite exhibits high activity and selectivity for light alkane dehydroaromatization, with Ga3+ sites playing a crucial role. The enhanced activity of Ga/H-MFI is attributed to cooperative effects between Ga3+ sites and Bronsted acid protons.
Article
Chemistry, Multidisciplinary
Brooke Soobrian, Alex J. King, Justin C. Bui, Adam Z. Weber, Alexis T. Bell, Frances A. Houle
Summary: Artificial photosynthesis is a promising method to produce commodity chemicals using abundant chemical feedstocks and renewable energy sources. However, affordable and effective hands-on activities for primary school students to demonstrate and teach artificial photosynthesis are lacking. Educating young students on this topic is crucial for developing a diverse next-generation energy workforce. This study confirms that an active learning-based lesson plan using cheap and accessible materials can effectively educate a broad range of young students on artificial photosynthesis, as demonstrated by the improved understanding of fifth grade students before and after the lesson plan.
JOURNAL OF CHEMICAL EDUCATION
(2023)
Article
Nanoscience & Nanotechnology
Alex J. King, Adam Z. Weber, Alexis T. Bell
Summary: A metal-insulator-semiconductor (MIS) structure is an attractive photoelectrode-catalyst architecture for promoting photoelectrochemical reactions, such as the formation of H2 by proton reduction. Understanding how the insulator layer determines the photovoltage and what properties lead to high photovoltages is critical to the development of MIS structures for solar-to-chemical energy conversion.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
John Safipour, Adam Z. Weber, Alexis T. Bell
Summary: Reactive carbon capture (RCC) is a promising solution for carbon capture and utilization. A systematic study found that RCC in aqueous environments is less effective and does not directly reduce into carbamate. Instead, the presence of amine solution suppresses the rate of CO formation while increasing that of H2.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Chanyeon Kim, Alex J. King, Shaul Aloni, Francesca M. Toma, Adam Z. Weber, Alexis T. Bell
Summary: Photoelectrochemical carbon-dioxide reduction (PEC CO2R) is a promising method for producing chemicals and fuels using sunlight, water, and carbon dioxide. However, the focus has been mostly on producing C-1 products, while the production of C2+ products has been rarely demonstrated. In this study, a Cu/TiO2/p-Si photocathode/catalyst structure was investigated to understand the effects of semiconductor-insulator interactions and illumination direction on the performance and product distribution. Coating the Cu surface with a thin bilayer of Sustainion/Nafion significantly enhanced the current density and faradaic efficiency to ethylene.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Multidisciplinary
Annette Bohme, Justin C. Bui, Aidan Q. Fenwick, Rohit Bhide, Cassidy N. Feltenberger, Alexandra J. Welch, Alex J. King, Alexis T. Bell, Adam Z. Weber, Shane Ardo, Harry A. Atwater
Summary: We investigated how the micrometer-scale morphology of a CO2R gas diffusion electrode (GDE) affects the mass transport properties and local CO2R performance. Using fluorescence confocal laser scanning microscopy (CLSM), we created local pOH maps around a copper GDE and observed that pOH decreases in microtrenches compared to the electrode surface. Multiphysics simulations correlated well with experimental measurements and suggested that the decreased pOH inside microcavities leads to enhanced selectivity towards multicarbon products. This study highlights the importance of a GDE's micromorphology on CO2R performance.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)