Article
Chemistry, Physical
Alan J. Barrios, Deizi Peron, Anoop Chakkingal, Achim Iulian Dugulan, Simona Moldovan, Kalthoum Nakouri, Joelle Thuriot-Roukos, Robert Wojcieszak, Joris W. Thybaut, Mirella Virginie, Andrei Y. Khodakov
Summary: This article investigated the reaction mechanism and efficient promoters for the CO2 hydrogenation to light olefins over iron catalysts using high throughput experimentation and extended characterization. It was found that alkaline metals were the most effective promoters, and simultaneous addition of potassium with other promoters further increased the selectivity to light olefins.
Article
Chemistry, Physical
Thongthai Witoon, Thanapha Numpilai, Khanin Nueangnoraj, Chin Kui Cheng, Metta Chareonpanich, Jumras Limtrakul
Summary: Recycling CO2 into light olefins is a promising method for reducing CO2 emissions. In this study, Fe-Co-K catalyst supported on different carbon materials were prepared and evaluated for CO2 hydrogenation to light olefins. The catalyst exhibited improved activity and selectivity towards light olefins due to enhanced metal dispersion and increased contact area. MMC support showed better performance in promoting olefins selectivity compared to MC support.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Review
Chemistry, Physical
Wenqi Liu, Sifan Cheng, Haripal Singh Malhi, Xinhua Gao, Zhenzhou Zhang, Weifeng Tu
Summary: This article discusses the thermodynamic overview of CO2 hydrogenation to olefins, the optimization of catalyst modifications, and current insights into the reaction mechanism. It also summarizes the current challenges and future trends in the field of CO2 hydrogenation to olefins.
Article
Chemistry, Physical
Thuy Ha Nguyen, Han Bom Kim, Eun Duck Park
Summary: CO2 methanation using ceria-supported cobalt catalysts with low cobalt contents was studied. The catalytic performance and physicochemical properties were influenced by the preparation method and treatment temperature. Among the catalysts tested, the ceria-supported cobalt catalyst prepared by wet impregnation method and calcined in air at 500 degrees C, then reduced in H-2 at 500 degrees C, showed the best catalytic performance.
Article
Chemistry, Physical
Chen Wang, Jianli Zhang, Xinhua Gao, Qingxiang Ma, Subing Fan, Tian-Sheng Zhao
Summary: The effects of oxygen vacancies (O-v) on the FeCx/ZnO catalyst for CO2 hydrogenation to linear alpha-olefins (LAOs) are investigated in this study. It is found that an appropriate concentration of O-v can enhance the CO2 conversion and LAOs selectivity. The increase in surface C/H ratio due to O-v also promotes the formation of key intermediates, but excessive O-v accelerates secondary hydrogenation.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Zhiqiang Zhang, Haoren Yin, Guangde Yu, Shun He, Jincan Kang, Zhiming Liu, Kang Cheng, Qinghong Zhang, Ye Wang
Summary: The Na- and Zn-promoted iron catalyst efficiently converts CO2 and CO into C-2 olefins with high selectivity and space-time yield, where ZnO facilitates the reverse water-gas shift reaction, chi- Fe5C2 catalyzes CO hydrogenation, and Na+ suppresses olefin hydrogenation. The close proximity between ZnO and chi-Fe5C2 plays a key role in the conversion of CO2 to olefins.
JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Physical
Haiyan Yang, Yaru Dang, Xu Cui, Xianni Bu, Jiong Li, Shenggang Li, Yuhan Sun, Peng Gao
Summary: This study fabricated zinc- and sodium-modulated iron catalysts, which exhibited the best activity and stability. Copper was found to decrease the energy barrier of the rate-determining step for olefin hydrogenation and result in a lower olefin-to-paraffin ratio. The ZnO/Fe5C2 interface facilitated olefin desorption and inhibited the undesirable secondary reaction of olefins, enabling a high selectivity.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Energy & Fuels
Yufang Bian, Chunying Xu, Xueying Wen, Leilei Xu, Yan Cui, Shuhan Wang, Cai-e Wu, Jian Qiu, Ge Cheng, Mindong Chen
Summary: A series of CeO2 supports with various morphologies were successfully fabricated and utilized as the supports of Ni-based CO2 methanation catalysts. The catalyst supported on CeO2 nanoparticles exhibited higher catalytic activity and better stability. By precisely designing the morphology of the CeO2 support, the catalytic performance of the Ni/CeO2 catalysts could be optimized.
Article
Chemistry, Physical
Pratya Promchana, Kittisak Choojun, Wanwisa Limphirat, Yingyot Poo-arporn, Tawan Sooknoi
Summary: Acetylene in ethylene-rich feed can be removed via acetylene/ethylene cross-metathesis over WO3-supported catalysts at 450 degrees C, yielding 1,3-butadiene with cyclohexene as a minor product. The catalyst must be treated with ethylene at 600 degrees C to generate a genuinely active site of tungsten (IV) alkylidene species (W=CH2). The H2 treatment decreases surface W--O concentration, and hence the activity.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Chemistry, Physical
Vanessa Lebarbier Dagle, Gregory Collinge, Mohammed Rahmana, Austin Winkelman, Wenda Hu, Jian Zhi Hu, Libor Kovarik, Mark Engelhard, Jennifer Jocz, Yong Wang, Mal-Soon Lee, Vassiliki-Alexandra Glezakou, Debmalya Ray, Roger Rousseau, Robert Dagle
Summary: This study reports on a Cu/ZrO2/SBA-16 catalyst with remarkable olefins selectivity and enhanced stability compared to the Ag/ZrO2/SBA-16 catalyst. Replacing Ag with Cu shifts the reaction pathway of crotonaldehyde hydrogenation, leading to the formation of butyraldehyde. Experimental and computational tools were used to verify the performance and stability advantage of the Cu/ZrO2/SBA-16 catalyst.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Engineering, Environmental
Humair Ahmed Baloch, Sabzoi Nizamuddin, M. T. H. Siddiqui, Sajid Riaz, Kristina Konstas, N. M. Mubarak, M. P. Srinivasan, G. J. Griffin
Summary: The study demonstrated that upgrading bio-oil in sub-supercritical ethanol using Pt/AC and Pd/AC as catalysts is effective, reducing acid fractions, increasing solution pH, and improving the heating value of the bio-oil.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2021)
Article
Polymer Science
Oleg Davydovich, Andrew J. Greenlee, Harrison D. Root, Annika L. Jansen, Shantae C. Gallegos, Matthew J. Warner, Michael S. Kent, Jorge A. Cardenas, Leah N. Appelhans, Devin J. Roach, Brad H. Jones, Samuel C. Leguizamon
Summary: Frontal polymerization is a method to rapidly generate high-performance polymeric materials through the propagation of a thermally driven polymerization wave. Encapsulated catalysts can provide remarkable latency to frontal polymerization systems, addressing the issue of poor storage lives caused by highly reactive catalysts.
Article
Chemistry, Multidisciplinary
Thalita S. Galhardo, Adriano H. Braga, Bruno H. Arpini, Janos Szanyi, Renato Goncalves, Bruno F. Zornio, Caetano R. Miranda, Liane M. Rossi
Summary: Control of the selectivity of CO2 hydrogenation catalysts is a fundamental challenge. In this study, it was found that changing the surface of a common Ni catalyst can lead to high selectivity toward CO formation in CO2 hydrogenation processes, representing an important step towards high-added-value products.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Physical
Heng Zhang, Anliang Dong, Bing Liu, Jie Chen, Yuebing Xu, Xiaohao Liu
Summary: Fischer-Tropsch synthesis is important for converting syngas into value-added fuels and chemicals. This study investigated the effect of hydrogen spillover on the catalytic performance of carbon nanotube-supported cobalt catalysts. It was found that larger cobalt particles resulted in higher catalytic activity and lower methane selectivity due to weaker atomic hydrogen spillover, while smaller cobalt particles led to lower catalytic activity and increased methane selectivity due to unstable surface hydrogen species distribution. The absence of surface defects in SiO2-supported cobalt catalysts resulted in lower and stable methane selectivity.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Alexander I. Nikiforov, Andrey G. Popov, Evgeny A. Chesnokov, Irina I. Ivanova
Summary: The supported MoO3/Al2O3-F catalysts were synthesized and characterized. The fluorination of support leads to an increase in the strength of Lewis Acid Sites and residual bridging OH groups, which enhances the propylene metathesis reaction. The results demonstrate the importance of support acidity in the catalytic process.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Nicola Bragato, Alvise Perosa, Maurizio Selva, Giulia Fiorani
Summary: A series of dihydroxybenzene-derived ILs were synthesized in a halide-free, eco-friendly manner and fully characterized. The most active catalyst for CO2 insertion into terminal epoxides to synthesize cyclic organic carbonates (COCs) was found to be methyltrioctylammonium hydroquinolate, [N-1888][HYD], under the proposed optimized conditions ([N-1888][HYD] 10% mol, T=120 degrees C, t=6 h, p(0)(CO2)=2.0 MPa, 12 examples, conversion >99%, yield up to 98%). Interestingly, [N-1888][HYD] also showed activity as a catalyst for CO2 insertion reactions with cyclohexene oxide (CHO), resulting in the formation of both COC and polycarbonate products. It is suggested that the catalytically active species for p(0)(CO2)>= 1.0 MPa is the hemicarbonate derivative of the hydroquinolate anion, which acts through an unusual hemicarbonate-alkoxide pathway for epoxide ring opening.
Article
Chemistry, Physical
Daniele Polidoro, Daily Rodriguez-Padron, Alvise Perosa, Rafael Luque, Maurizio Selva
Summary: Chitin, a renewable carbon and nitrogen source, is the second most abundant biopolymer on Earth after cellulose. This study successfully prepared chitin-derived N-doped carbonaceous materials functionalized with palladium metal nanoparticles. The physicochemical properties of these nanocomposites were investigated using a multi-technique approach, and their catalytic activity in reductive amination reactions was explored. Specifically, a biomass-derived platform molecule, furfural, was transformed into valuable bi-cyclic compounds under continuous flow conditions.
Article
Chemistry, Multidisciplinary
Daniele Polidoro, Irina Elena Mihai, Alvise Perosa, Maurizio Selva
Summary: Various multiphase systems consisting of immiscible liquid water, a hydrocarbon, and an ionic liquid were studied for the hydrogenation/hydrolysis of 5-hydroxymethylfurfural. A liquid triphase system composed of water, isooctane, and methyltrioctylammonium chloride achieved excellent selectivity control with high yields of the desired product. By separating the reagents and catalyst in different phases, the catalyst could be effectively recycled and reused multiple times without any loss of activity or selectivity.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Physical
Carlotta Campalani, Guillaume Petit, Jean-Christophe M. Monbaliu, Maurizio Selva, Alvise Perosa
Summary: Bass-CDs, synthesized from fishery waste, were used as a cheap and readily available photocatalyst in combination with oxygen and UV light for the efficient degradation of azo dyes. Both batch and continuous flow conditions were studied, and all the azo dyes were fully degraded, highlighting the suitability of bass-CDs for wastewater decontamination.
Article
Chemistry, Multidisciplinary
Davide Rigo, Daniele Polidoro, Lorenzo Marcuzzo, Alvise Perosa, Maurizio Selva
Summary: Isopropenyl acetate (iPAc) can convert refined and crude glycerol (CG) into valuable products, such as allyl acetate, triacetin (TA), and acetal acetates, under continuous-flow conditions. This study presents two novel tandem catalytic protocols that achieve high yields of these products by using a combination of innocuous compounds with different roles. The importance of this research lies in providing a green and efficient method for the chemical upgrading of glycerol into valuable products, and improving the yields by optimizing process variables and catalyst selection.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Daniele Polidoro, Giancarmelo Stamilla, Matteo Feltracco, Andrea Gambaro, Alvise Perosa, Maurizio Selva
Summary: A single-step protocol for hydrolytic hydrogenation of microcrystalline cellulose into sorbitol was developed using commercial carbon-supported Ru as a catalyst, with gaseous CO2 as an acid source and molecular hydrogen as a reductant. By adjusting reaction parameters, such as temperature, time, and pressure, cellulose conversion of 81% was achieved at 220°C in 18 hours under 30 and 40 bar of H2 and CO2, respectively.
Article
Chemistry, Physical
Daniele Polidoro, Alina M. Balu, Maurizio Selva, Rafael Luque, Sameh M. Osman, Tripti Chhabra
Summary: Microwave (MW) and conventional heating (CH) methods were compared for the synthesis of fuel additives from levulinic acid. Phosphomolybdic acid (PMA) and phosphotungstic acid (PTA)-containing graphitic carbon nitride (GCN) were synthesized and optimized to achieve high yields. MW significantly reduced reaction times and is a more sustainable approach for the synthesis of various fuel additives. Scale-up experiments showed that MW with optimum GCN-PMA achieved higher productivity compared to CH conditions.
SUSTAINABLE ENERGY & FUELS
(2023)
Article
Chemistry, Multidisciplinary
Nicola Bragato, Alvise Perosa, Maurizio Selva, Giulia Fiorani, Roberto Calmanti
Summary: In this study, the syntheses, characterisation, properties comparison, and applications of molybdate and polyoxomolybdate ionic liquids as bifunctional catalysts for CO2 insertion into epoxides were described. The synthetic methods relied on anion exchange and acid-base reactions, including a novel route for the synthesis of molybdate ionic liquids using a halide-free organic precursor. The investigations showed that tetrabutylammonium molybdate could serve as an efficient catalyst for the production of hexane carbonate from 1,2-epoxyhexane under solventless and halide-free conditions.
Review
Chemistry, Multidisciplinary
Giulia Fiorani, Alvise Perosa, Maurizio Selva
Summary: This review provides a comprehensive analysis of the reactions and applications of various organic carbonates and enol esters for the functionalization and upgrading of renewable compounds. Five sections cover the synthetic methods of organic carbonates, their reactions as alkylating, carboxylating, and acylating agents, and their use as solvents. The review also discusses the pros and cons of different methods and suggests areas for future research and analysis.
Article
Chemistry, Multidisciplinary
Xuemei Liu, Chaonan Cui, Shuoshuo Wei, Jinyu Han, Xinli Zhu, Qingfeng Ge, Hua Wang
Summary: This study presents a new strategy for designing efficient photocatalysts that can convert CO2 into hydrocarbons by utilizing synergistic catalytic sites. The findings provide a solution for the selective photocatalytic reduction of CO2 to CH4.
Article
Chemistry, Multidisciplinary
Chengxian Hu, Dan Wang, Lu Wang, Ying Fu, Zhengyin Du
Summary: A novel one-pot, three-component reaction conducted under electrochemical conditions was studied. The reaction involved 2-aminothiophenols, aldehydes, and malononitrile, using TBABF4 as an electrolyte and CuI as a catalyst. The proposed reaction mechanism suggested that CuI served as an electron relay. This method offers simplified operation, high atom economy, and mild reaction conditions.
Article
Chemistry, Multidisciplinary
Zhi Yang, Yu Chen, Linxi Wan, Yuxiao Li, Dan Chen, Jianlin Tao, Pei Tang, Fen-Er Chen
Summary: A highly enantioselective method for the complete hydrogenation of pyrimidinium salts using Ir/(S,S)-f-Binaphane complex as the catalyst was developed. This method provides easy access to fully saturated chiral hexahydropyrimidines, which are prevalent in many bioactive molecules. The reactions exhibit high yields and enantioselectivities under mild reaction conditions without additives. Successful application of this methodology in a continuous flow fashion further extends its practical utility.
Article
Chemistry, Multidisciplinary
Tina Jeoh, Jennifer Danger Nill, Wujun Zhao, Sankar Raju Narayanasamy, Liang Chen, Hoi-Ying N. Holman
Summary: In this study, the enzymatic hydrolysis of cellulose was investigated using real-time infrared spectromicroscopy. The spatial heterogeneity of cellulose was found to impact the hydrolysis kinetics. Hydration affected cellulose ordering, and Cel7A preferentially removed less extensively hydrogen bonded cellulose.
Article
Chemistry, Multidisciplinary
Tiphaine Richard, Walid Abdallah, Xavier Trivelli, Mathieu Sauthier, Clement Dumont
Summary: An effective method of grafting functionalities onto lignin based on glycerol carbonate has been developed using an efficient nickel-catalysed telomerisation reaction. This method allows lignin to have new reactive functions and reduces the glass transition temperatures of modified lignins, thereby expanding the application range of lignin-based resins.
Article
Chemistry, Multidisciplinary
Jing Qi, Xiyan Wang, Gan Wang, Srinivas Reddy Dubbaka, Patrick ONeill, Hwee Ting Ang, Jie Wu
Summary: This study presents a green and environmentally friendly approach for the synthesis of imides using electrocatalytic oxidation with H2O as the oxygen source. The method eliminates the need for toxic or expensive oxidants and achieves high yields under mild reaction conditions. It shows broad substrate compatibility and potential for industrial applications.
Article
Chemistry, Multidisciplinary
Babasaheb Sopan Gore, Lin-Wei Pan, Jun-Hao Lin, Yi-Chi Luo, Jeh-Jeng Wang
Summary: Here, we report a visible light-promoted intramolecular radical cascade reaction for the construction of fluorenol and naphthalene-fused cyclopropyl carbaldehyde derivatives. This method offers mild reaction conditions, a broad substrate scope, excellent step efficiency, and scalability, without the need for external chemical oxidants. The novelty of this protocol was demonstrated by synthesizing chrysene analogs and performing late-stage functionalizations.
Article
Chemistry, Multidisciplinary
Juho Antti Sirvio, Idamaria Romakkaniemi, Juha Ahola, Svitlana Filonenko, Juha P. Heiskanen, Ari Ammala
Summary: This article discusses the method of using supramolecular interaction between an aromatic hydrogen bond donor and lignin to achieve rapid delignification of softwood at low temperatures.
Article
Chemistry, Multidisciplinary
Yunyan Meng, Chunxiang Pan, Na Liu, Hongjiang Li, Zixiu Liu, Yao Deng, Zixiang Wei, Jianbin Xu, Baomin Fan
Summary: A novel visible light-driven synthesis method for 2,3-diamines has been developed, which has mild conditions, avoids the use of metal reagents, and can synthesize diamines and diols in one pot.
Article
Chemistry, Multidisciplinary
Mingqing Huang, Haiyang Huang, Mengyao You, Xinxin Zhang, Longgen Sun, Chao Chen, Zhichao Mei, Ruchun Yang, Qiang Xiao
Summary: A direct air-oxidized strategy for the synthesis of benzo[b]phosphole oxides was developed in this study. Arylphosphine oxides were transformed into phosphinoyl radicals, which were further combined with various alkynes to achieve the desired products. DFT calculations revealed the mechanism of phosphinoyl radical formation.
Article
Chemistry, Multidisciplinary
Anwei Wang, Jiayin Huang, Chunsheng Zhao, Yu Fan, Junfeng Qian, Qun Chen, Mingyang He, Weiyou Zhou
Summary: This study demonstrates an innovative strategy for the aerobic oxidation of C(sp(3))-H bonds using gamma-valerolactone. By optimizing the reaction conditions and utilizing specific catalysts, efficient oxidation of C(sp(3))-H bonds is achieved with good chemoselectivity in certain cases.
Article
Chemistry, Multidisciplinary
Shun Li, Likai Tong, Zhijian Peng, Bo Zhang, Xiuli Fu
Summary: Sulfide compounds show promise as electrocatalysts for water splitting, but their performance is limited by factors such as limited active sites and hindered substance transport. This study successfully prepared a high-entropy sulfide (ZnCoMnFeAlMg)(9)S-8, which reduced grain size and increased specific surface area, enabling the realization of a dual-functional catalyst with multiple catalytic sites. High entropy also modulated the electronic properties of sulfides, reducing the potential energy barrier for hydrolysis. This research introduces a new approach for functionalizing high entropy nanomaterials and improves the performance of water splitting catalysts.