Article
Chemistry, Multidisciplinary
Xuechen Xu, Cheng-Bin Hong, Haichao Liu
Summary: We report a novel route to the sustainable synthesis of 5-Methyl-2-furancarboxylic acid (MFA) from bio-renewable 5-hydroxymethyl-2-furancarboxylic acid (HMFA) through the direct cleavage of the C-OH bond in HMFA at ambient temperature. Pd catalysts supported by active carbon (C) exhibited high efficiency and stability in the hydrogenolysis of HMFA to MFA, providing a high yield of 94.5%. This work provides an efficient strategy for the selective cleavage of the alpha-C-OH bonds in the furan ring and the sustainable production of MFA and its derivatives from biomass resources.
Article
Chemistry, Physical
Linxiao Chen, Julia B. Moreira, Laura C. Meyer, Janos Szanyi
Summary: This study reports an efficient polypropylene (PP) hydro-conversion process using a novel, highly active Ru and Ni supported on a sol-gel anatase TiO2 catalyst. Mechanistic studies revealed that the strong polymer-catalyst interaction and abundant 3C accelerated isomerization and sequential β-scission reactions, leading to the selective formation of high-valued C4-20 products. The findings contribute to the development of a noble-metal-free catalyst for plastic waste upcycling.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Linxiao Chen, Laura C. Meyer, Libor Kovarik, Debora Meira, Xavier Pereira-Hernandez, Honghong Shi, Konstantin Khivantsev, Oliver Y. Gutierrez, Janos Szanyi
Summary: This study discovers that low-loading Ru/CeO2 exhibits remarkable catalytic performance in the hydrogenolysis of polyolefin plastics, with high conversion efficiency, low selectivity toward CH4, and good isomerization ability. The catalytic behavior changes coincide with the transition from well-defined to highly disordered Ru species in the low-loading range.
Article
Chemistry, Multidisciplinary
Bin Hu, Lisa Warczinski, Xiaoyu Li, Mohong Lu, Johannes Bitzer, Markus Heidelmann, Till Eckhard, Qi Fu, Jonas Schulwitz, Mariia Merko, Mingshi Li, Wolfgang Kleist, Christof Hattig, Martin Muhler, Baoxiang Peng
Summary: This study demonstrates an efficient method for the hydrogenolysis of HMF to DMF under mild reaction conditions using Pd nanoparticles supported on N-containing and N-free mesoporous carbon materials, along with formic acid (FA) and hydrogen. It was found that the main role of FA is to shift the dominant reaction pathway from the hydrogenation of the aldehyde group to the hydrogenolysis of the hydroxymethyl group, thereby significantly enhancing the reaction rate. The interaction between Pd2+ species and pyridine-like N atoms was shown to enhance the selective hydrogenolysis of the C-OH bond in the presence of FA, leading to the stabilization of H-.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Ge Meng, Wu Lan, Lilong Zhang, Shibin Wang, Tanhao Zhang, Shuo Zhang, Ming Xu, Yu Wang, Jian Zhang, Fengxia Yue, Yulong Wu, Dingsheng Wang
Summary: A synergistic catalyst (Mo1Al/MgO) combining atomically dispersed Mo centers and Al Lewis acid sites on a MgO substrate was designed for the depolymerization of Eucalyptus lignin. The Mo1Al/MgO achieved a near-theoretical monophenol yield of 46% and a high selectivity of 92% for coniferyl and sinapyl methyl ether, with good cycling durability, in an inert N-2 atmosphere. This study confirms the feasibility of designing better-performing catalysts with synergistic multiactive sites for the efficient and selective disassembly of complex renewable biopolymers into highly value-added products with lower cost and greater security.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Mingyu Chu, Xianpeng Wang, Xuchun Wang, Xiangxi Lou, Congyang Zhang, Muhan Cao, Lu Wang, Youyong Li, Sibao Liu, Tsun-Kong Sham, Qiao Zhang, Jinxing Chen
Summary: Catalytic hydrogenolysis of end-of-life polyolefins can produce value-added liquid fuels, and researchers have discovered that using Ru single-atom catalyst can effectively suppress methanation, leading to higher fuel yields. The Ru single-atom catalyst supported on CeO2 showed an ultralow CH4 yield of 2.2% and a liquid fuel yield of over 94.5% at 250 degrees C for 6 hours. This breakthrough offers promising opportunities for plastic upcycling.
Article
Engineering, Environmental
Wen-Huan Huang, Xi-Ming Li, Xiu-Fang Yang, Hai-Yang Zhang, Pan-Bo Liu, Yang-Min Ma, Xing Lu
Summary: The mesoporous CoS/MoS2 polyhedron embedded with CeO2 nanoparticles showed enhanced OER electrocatalytic performance in alkaline conditions, with CeO2@CoS/MoS2 catalyst displaying excellent stability and performance.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Energy & Fuels
Wenqi Zhao, Xiaowei Bai, Xiangrui Lin, Yalkunjan Tur Sun, Mei Zhong, Zhenghua Dai, Jian Li
Summary: In this study, a green co-precipitation-hydrothermal method was used to prepare Ni-La(OH)3 catalysts, which achieved high conversion and selectivity of 1,5-pentanediol from THFA under mild conditions. The key role of the La(OH)3 phase, basic sites, and the Nin+-O-La3+ structure in promoting the selective hydrogenolysis and ring opening of THFA was elucidated. Additionally, the co-dehydrogenation of secondary alcohols was demonstrated to lower reaction pressure and extend catalyst lifetime. This work provides a sustainable and environmentally friendly approach for the production of 1,5-pentanediol from biomass-based furfural and its derivatives, with potential applications in polymer synthesis and green chemistry.
Article
Materials Science, Biomaterials
Yu Huang, Zewei Wang, Guiju Zhang, Jie Ren, Li Yu, Xuhan Liu, Yuanxi Yang, Abirami Ravindran, Chloe Wong, Rongjun Chen
Summary: A novel pH/redox-dual responsive nanoemulsion-embedded composite hydrogel was synthesized for efficient oral delivery and controlled intestinal release of ions, showing good biocompatibility and the ability to release magnesium ions efficiently in the neutral and reducing intestinal environment.
JOURNAL OF MATERIALS CHEMISTRY B
(2021)
Article
Chemistry, Physical
Yan Chen, Yang Zeng, Chin-Te Hung, Zhenghao Zhang, Zirui Lv, Senchuan Huang, Yi Yang, Yupu Liu, Wei Li
Summary: In this study, hollow mesoporous Pt/WOxSiO2-TiO2 nanosphere catalysts with bi-functional interfaces were synthesized for efficient conversion of glycerol to 1,3-propanediol. The catalysts showed high selectivity and stability, delivering a favorable 1,3-PDO yield of 45.7%. This work provides a new strategy for the synthesis of catalysts with high selectivity, activity, and stability.
Article
Chemistry, Physical
Zhongnan Gao, Dongyue Zhao, Qingpeng Cheng, Dejian Zhao, Yuexi Yang, Ye Tian, Tong Ding, Song Song, Lihong Guo, Xingang Li
Summary: The mesoporous SiO2-encapsulated nano-Co3O4 catalyst, with unique pitaya-like structure, exhibits high CO oxidation activity and thermal stability. It can be effectively regenerated, improves cobalt resources utilization efficiency, and is suitable for practical applications.
Article
Chemistry, Multidisciplinary
Yanzhi Wang, Hao Lv, Lizhi Sun, Ben Liu
Summary: Mesoporous metal-metalloid/nonmetal alloys have attracted increasing attention as highly efficient nanocatalysts due to their ability to enhance precious noble metal utilization efficiency, accelerate transfer processes, introduce new functionalities, optimize metal sites, and enhance catalytic activity and stability. Research in this area also addresses the challenges in synthesizing and applying mesoporous noble metal-metalloid/nonmetal alloys.
Article
Chemistry, Physical
Xincong Lv, Shengming Yin
Summary: A highly efficient non-precious catalyst consisting of cobalt (Co) species embedded nitrogen (N) and phosphorus (P) co-doped carbon nanotubes (CNT) was successfully fabricated for hydrogen evolution reaction (HER) at low overpotentials. The catalyst exhibited excellent activity and stability, making it one of the best electrocatalysts in acidic electrolytes.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Julia C. Steinbach, Fabio Fait, Hermann A. Mayer, Andreas Kandelbauer
Summary: Mesoporous silica microspheres (MPSMs) were synthesized using a hard template method to control particle size and pore properties. Response surface methodology was applied to predict the effects of synthesis parameters on MPSM characteristics. The prepared MPSMs were successfully applied as stationary phase for reversed-phases liquid chromatography, achieving protein and amino acid separation.
Article
Engineering, Environmental
Xinyun Yao, Bei Yu, Yinghao Xue, Xianqiang Ran, Jiaqi Zuo, Kaipei Qiu
Summary: The study designed a high-performance copper-nickel alloy embedded mesoporous carbon electrocatalyst, achieving complete conversion of NO3- in the absence of Cl- and 100% selectivity towards N2 in the presence of Cl-. Density functional theory calculations confirmed that the incorporation of Ni atoms into the Cu interface significantly improved the adsorption of intermediates, reducing the barrier for hydrogenation and ensuring high efficiency.
JOURNAL OF WATER PROCESS ENGINEERING
(2021)
Article
Nanoscience & Nanotechnology
Xingyi Lyu, Max Meirow, Xun Wu, Xinwei Zhou, Yuzi Liu, Wenyu Huang, Tao Li, Byeongdu Lee
Summary: The mesoporous silica shell coating the hydrogenolysis nano-catalyst alters the molecular weight distributions of cleaved polymer chains compared to catalysts without a shell. The shell reduces low-valued gaseous products and increases the median molecular weight of the product, enhancing the value of the products for polymer upcycling. The spatial distribution of polystyrene chains in the nanochannels reveals a non-uniform distribution for longer chains.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Alexander Volkov, Jiashan Mi, Kanika Lalit, Puranjan Chatterjee, Dapeng Jing, Scott L. Carnahan, Yunhua Chen, Simin Sun, Aaron J. Rossini, Wenyu Huang, Levi M. Stanley
Summary: The library of imine-linked covalent organic frameworks (COFs) has significantly expanded in the past two decades, offering a wide range of morphologies, pore sizes, and applications. While various synthetic methods have been developed to enhance COF functionalities, most of them are specific to certain applications. This study presents a general strategy to introduce functional group handles in COFs through the Ugi multicomponent reaction, enabling the functionalization of any COFs containing imine linkages.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Polymer Science
Tommy Yunpu Zhao, Max Meirow, Akalanka Tennakoon, Xun Wu, Alexander L. L. Paterson, Long Qi, Anne M. M. LaPointe, Jessica V. V. Lamb, Takeshi Kobayashi, Massimiliano Delferro, Aaron D. D. Sadow, Wenyu Huang, Erik Luijten, Frederic A. Perras
Summary: Chemical polymer upcycling by processive catalysts is a promising strategy for plastic waste remediation, which can produce high-value products with minimal energy input. By using a novel processive catalyst with a mesoporous SiO(2) shell/Pt nanoparticle/SiO2 core architecture, we found that the deconstruction of polyolefins occurs within narrow pores and involves a dehydrogenation-rehydrogenation cycle. The porous architecture enables the catalyst to perform multiple successive cleavages to the same polymer chain, and the extent of processivity is strongly correlated with the length of the pores.
Article
Chemistry, Physical
Shaojiang Chen, Akalanka Tennakoon, Kyung-Eun You, Alexander L. L. Paterson, Ryan Yappert, Selim Alayoglu, Lingzhe Fang, Xun Wu, Tommy Yunpu Zhao, Michelle P. P. Lapak, Mukunth Saravanan, Ryan A. A. Hackler, Yi-Yu Wang, Long Qi, Massimiliano Delferro, Tao Li, Byeongdu Lee, Baron Peters, Kenneth R. R. Poeppelmeier, Salai C. C. Ammal, Clifford R. R. Bowers, Frederic A. Perras, Andreas Heyden, Aaron D. D. Sadow, Wenyu Huang
Summary: Non-reducible zirconia catalysts can efficiently hydrogenolytically cleave polyolefins, achieving similar activity as precious metal nanoparticles.
Article
Nanoscience & Nanotechnology
Hengzhou Liu, Jiaqi Yu, Yifu Chen, Jungkuk Lee, Wenyu Huang, Wenzhen Li
Summary: Electrocatalytic oxidative dehydrogenation (EOD) of aldehydes allows for the production of bipolar H-2 at ultra-low voltage with carboxylic acid co-generation. This study presents a simple galvanic replacement method to prepare CuM (M = Pt, Pd, Au, and Ag) bimetallic catalysts, enabling industrially relevant current densities in the EOD of furfural. The incorporation of noble metals onto the Cu surface and the subsequent enlargement of its surface area significantly improve the EOD performance, with CuPt achieving a record-high current density of 498 mA cm(-2) and a Faradaic efficiency of >80% to H-2 at a low cell voltage of 0.6 V. Further research is required to understand the synergistic effects of Cu-M on furfural EOD and enhance the catalyst stability, thus facilitating the future production of green hydrogen and carbon chemicals with practical rates and low-carbon footprints.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Akalanka Tennakoon, Xun Wu, Max Meirow, Daniel Howell, Jarod Willmon, Jiaqi Yu, Jessica V. Lamb, Massimiliano Delferro, Erik Luijten, Wenyu Huang, Aaron D. Sadow
Summary: By embedding active platinum nanoparticles between linear, hexagonal mesoporous silica and gyroidal cubic MCM-48 silica, the new catalyst design emphasizes the pore effect and selectively deconstructs polyolefins into valuable hydrocarbon chains while generating minimal volatile byproducts, including methane.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Normanda Brown, Ziad Alsudairy, Ranjan Behera, Fazli Akram, Kuangcai Chen, Kayla Smith-Petty, Bria Motley, Spirit Williams, Wenyu Huang, Conrad Ingram, Xinle Li
Summary: In this study, a green and efficient liquid-assisted mechanochemical synthesis method was used to successfully prepare covalent organic framework (COF) adsorbents with high iodine capture capacity. The synthesis method yielded six COFs with diverse pore sizes and functionalities in just 1 hour using ball milling and liquid additives at ambient temperature. One of the COFs achieved high crystallinity and a remarkable surface area of 1387 m(2) g(-1) in just 1 minute of ball milling. Four of the mechanochemically synthesized COFs exhibited outstanding iodine adsorption capacities of 6.4-7.1 g g(-1) at 75°C, comparable to or exceeding those of solvothermally synthesized COF and most reported COF adsorbents. Fourier transform infrared and X-ray photoelectron spectroscopy confirmed the charge transfer between iodine and COF adsorbents. This mechanochemical methodology opens up a new pathway for green, rapid, facile, and scalable synthesis of COFs, with great prospects in environmental remediation and other applications.
Article
Chemistry, Multidisciplinary
Jacklyn N. Hall, A. Jeremy Kropf, Uddhav Kanbur, Fulya Dogan, Carly Byron, Jianguo Wen, Massimiliano Delferro, David M. Kaphan
Summary: Isolated Pd atoms supported on high surface area MnO2, prepared by oxidative grafting, catalyze the low temperature oxidation of CO with results of spectroscopic characterization indicating a synergistic role of Pd and MnO2 in facilitating redox turnovers.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Frederic A. Perras, Alejandra Arroyave, Scott A. Southern, Jessica V. Lamb, Yuting Li, Anne LaPointe, Massimiliano Delferro
Summary: By using O-17-enriched supports, highly informative multidimensional NMR experiments, including radial and vertical distance measurements, can be conducted to elucidate the geometry of surface organometallic complexes.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Tianlei Li, Hengzhou Liu, Jiaqi Yu, Yifu Chen, Wenyu Huang, Wenzhen Li
Summary: In this study, a MOF-derived Co3O4/nitrogen-doped carbon composite (Co3O4/NC) prepared through a two-step calcination method exhibited higher activity than a commercial RuO2 catalyst in the electrolysis of chlorate, which can be attributed to its higher specific surface area and lower resistance. Furthermore, the Co3O4/NC maintained stable potential and high faradaic efficiency throughout the 10-hour electrolysis test.
Article
Chemistry, Multidisciplinary
Gourab Bhaskar, Ranjan K. Behera, Volodymyr Gvozdetskyi, Scott L. Carnahan, Raquel A. Ribeiro, Paul Oftedahl, Charles Ward, Paul C. Canfield, Aaron J. Rossini, Wenyu Huang, Julia V. Zaikina
Summary: Doping is an effective method to modify the structure and properties of compounds. In this study, the substitution of Ni with Co in layered LiNiB compounds was found to stabilize the high-temperature phase and result in a new structural motif. The doped LiNi0.7Co0.3B compound exhibited different reactions under ambient and anaerobic conditions, and showed excellent catalytic performance.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Max Meirow, Akalanka Tennakoon, Xun Wu, Jarod Willmon, Daniel Howell, Wenyu Huang, Aaron D. Sadow, Erik Luijten
Summary: Due to the plastic waste crisis, selective chemical upcycling of polyolefins into value-added products has attracted great interest. A recent study has synthesized a catalytic architecture that can control the product chain lengths by manipulating the pore length, and uncovered the dynamic phenomenon responsible for the pore-length dependence of the cleavage products.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Yeongseo An, Puranjan Chatterjee, Pranjali Naik, Sayak Banerjee, Wenyu Huang, Igor I. Slowing, Vincenzo Venditti
Summary: Substrate-support interactions play an important role in the hydrogenation of phenolic compounds. Titanium oxide has the ability to form hydrogen bonds with the substrate and mediate the addition of activated hydrogens.
Article
Chemistry, Multidisciplinary
William S. Salvia, Tommy Yunpu Zhao, Puranjan Chatterjee, Wenyu Huang, Frederic A. Perras
Summary: The study confirmed that the active sites in amorphous silica-alumina are zeolitic bridging Bronsted sites, using selective isotope labeling and quantitative NMR distance measurements.
CHEMICAL COMMUNICATIONS
(2023)