Review
Biotechnology & Applied Microbiology
Ranjith Kumar Kankala, Ya-Hui Han, Hong-Ying Xia, Shi-Bin Wang, Ai-Zheng Chen
Summary: Mesoporous silica nanoparticles (MSNs) have great potential in biomedical applications, but traditional MSNs have limitations such as reduced drug encapsulation efficacy and poor degradability. Hierarchically-engineered MSNs have been developed by tuning the pore sizes, modifying the surfaces, and engineering the siliceous networks. These engineered MSNs have complex structures and can be applied in drug delivery, bioimaging, tissue engineering, and other fields.
JOURNAL OF NANOBIOTECHNOLOGY
(2022)
Article
Chemistry, Inorganic & Nuclear
Israel T. Pulido-Diaz, Alejandro Serrano-Maldonado, Carlos Cesar Lopez-Suarez, Pedro A. Mendez-Ocampo, Benjamin Portales-Martinez, Aida Gutierrez-Alejandre, Karla P. Salas-Martin, Itzel Guerrero-Rios
Summary: The study demonstrates that nicotinamide groups grafted on ordered mesoporous silica (OMS) can serve as stabilizers for RhNPs used as catalysts, forming spherical rhodium nanoparticles with a narrow size distribution. On the contrary, amine-functionalized OMS tends to form RhNP aggregates after catalytic reactions, affecting the reaction efficiency. Supported RhNPs also exhibit selective reduction of different groups and show high activity in reductive amination reactions.
DALTON TRANSACTIONS
(2021)
Article
Chemistry, Physical
Meijia Li, Tianyu Zhang, Shi-Ze Yang, Yifan Sun, Junyan Zhang, Felipe Polo-Garzon, Kevin M. Siniard, Xinbin Yu, Zili Wu, Darren M. Driscoll, Alexander S. Ivanov, Hao Chen, Zhenzhen Yang, Sheng Dai
Summary: A mechanochemistry-driven approach was used to construct strong metal-support interactions (SMSIs) under neat and ambient conditions, resulting in enhanced catalysis. The encapsulation degree and overlayer structures could be customized, leading to improved hydrogenation activity.
Article
Chemistry, Physical
Lebohang Macheli, Emanuela Carleschi, Bryan P. Doyle, Gerard Leteba, Eric van Steen
Summary: Metal-support interactions in inverse catalysts prepared by adsorbing TEOS on Co3O4 can be manipulated by varying the solvent mixture. Deposition of TEOS on Co3O4 nanoparticles in n-hexane results in the formation of silica oligomers interacting strongly with cobalt(II,III)oxide after calcination at 573 K. Modification of Co3O4 nanoparticles with TEOS in a hydrolysing environment results in a stronger interaction due to the formation of surface cobalt silicate through hydrolysis.
JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Physical
Monika Kot, Robert Wojcieszak, Ewa Janiszewska, Mariusz Pietrowski, Michal Zielinski
Summary: Commercial silica modified with NH4F or NH4Cl salts and thermally treated can generate acidic sites and alter structural properties, along with additional porosity. NH4F solution leads to decreased specific surface area, increased pore diameter, and higher total acidity. The resulting acid sites' number and strength depend on the anion in the ammonium salt and concentration of the solution. The NH4F-modified silica supported iridium catalyst exhibits higher activity in toluene hydrogenation due to the generation of adsorption centers for toluene.
Article
Chemistry, Multidisciplinary
Sara Malekkhaiat Haffner, Elisa Parra-Ortiz, Kathryn L. Browning, Elin Jorgensen, Maximilian W. A. Skoda, Costanza Montis, Xiaomin Li, Debora Berti, Dongyuan Zhao, Martin Malmsten
Summary: The study showed that the topography of nanoparticles strongly influences their interaction with bacteria-mimicking lipid bilayers, especially in the presence of antimicrobial peptides. Virus-like mesoporous nanoparticles exhibit a more pronounced membrane disruption after loading with LL-37 compared to smooth nanoparticles.
Article
Materials Science, Ceramics
Eva Krakor, Sven Saniternik, Isabel Gessner, Robert Frohnhoven, Michael Wilhelm, Marco Drexelius, Nurgul Tosun, Ines Neundorf, Sanjay Mathur
Summary: Intensive and overuse of antibiotics have led to a rise in antibiotic resistance globally, creating a demand for alternative treatments. Metal ions like copper, silver, and zinc have been used to inhibit microorganism growth for centuries. This study focuses on the synthesis of metal and oxide nanoparticles immobilized on hollow mesoporous silica capsules (HMSCs) for efficient antimicrobial effects against both Gram-positive and Gram-negative bacteria. The results show promising potential for metal-loaded capsules as antibacterial delivery vehicles, providing sustained bacterial inhibition over several hours.
JOURNAL OF THE AMERICAN CERAMIC SOCIETY
(2022)
Article
Chemistry, Physical
Xiaohan Yuan, Tiancheng Pu, Mengwei Gu, Minghui Zhu, Jing Xu
Summary: This study systematically investigates a series of nickel-iron-based bimetallic catalysts to unveil the nature of active sites for the CO2 hydrogenation reaction, revealing an environmental-sensitive strong metal-support interaction between Ni nanoparticles and iron oxides. Iron oxides migrate and entirely cover the metallic Ni nanoparticles during the reaction, yielding a more active core-shell-type structure with much-improved reducibility, a process indirectly monitored in a time-resolved manner by in situ DRIFTS and confirmed to complete within 30 min of the reaction.
Article
Chemistry, Physical
Bin Wang, Shu-han Lu, Shi-yuan Wang, Pei-ya Li, Tao Fang
Summary: By studying three different Ru catalysts supported on zirconium-based supports, we have identified the effects of supported metal-support strong interaction (SMSI), metal-support anion interaction (MSAI) and hydrogen spillover on the hydrogenation reaction path and the occurrence of isomerization in 12H-NEC product.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Physical
Wang Ke, Xiangdong Qin, Robert M. Palomino, Juan Pablo Simonovis, Sanjaya D. Senanayake, Jose A. Rodriguez, Francisco Zaera
Summary: The redox properties of titania films grown by atomic layer deposition (ALD) on SBA-15 were investigated as a function of film thickness. Si-29 CP/MAS NMR and infrared absorption spectroscopy were used to determine the surface species formed during initial deposition and the transition from silica to titania surfaces. The reducibility of titania sites by CO and H-2 was studied ex situ using electron paramagnetic resonance (EPR) and in situ with ambient-pressure X-ray photoelectron spectroscopy (XPS). The results showed that the amorphous titania ALD films were more easily reduced and the reduction was reversible. The surface also exhibited a transition, with mixed Si-O-Ti sites forming in the early ALD cycles and a more typical titania surface developing as the film grew.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Review
Chemistry, Inorganic & Nuclear
Anandhu Mohan, Augustine Jaison, Young-Chul Lee
Summary: The regulation of a large amount of CO2 in the environment is crucial to prevent environmental catastrophes, and this can be achieved through efficient carbon capture and conversion into useful chemicals. Mesoporous silica nanoparticles (MSNs) are ideal support materials for heterogeneous catalysis due to their unique characteristics. This review discusses the functionalization of MSNs, the synthesis of MSN-based catalysts, and their potential applications in CO2 fixation reactions. It highlights the design of an ideal CO2 fixation catalyst, the addition of various functionalities to MSNs, and the effects of controlling particle size distribution, active species dispersion, and interactions between active species and supports. Furthermore, this review provides an overview of the key issues, current developments, and barriers in the field of MSN-based catalysts for CO2 fixation, along with proposed research goals and viable solutions for their implementation.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Multidisciplinary
Ruo-Can Qian, Ze-Rui Zhou, Weijie Guo, Yuting Wu, Zhenglin Yang, Yi Lu
Summary: The strategy based on DNAzymes allows for controllable cell-cell interactions triggered by metal ions, effectively manipulating cell behaviors such as cell-cell conjunctions and disaggregation. This method has been successfully applied to control assembly and disassembly between two cell spheroids.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Applied
Byeongju Song, Jeongmyeong Kim, Iljun Chung, Yongju Yun
Summary: The catalytic properties of Pt catalysts supported on mesoporous silica were studied in the enantio-selective hydrogenation of ethyl pyruvate. The results showed that the pore structure and size of the m-SiO2 supports significantly influenced both the activity and enantioselectivity. The use of specific modifiers and H-2 pressure further improved the performance of the catalysts.
Article
Chemistry, Physical
Jiadong Zhu, Diana Ciolca, Liang Liu, Alexander Parastaev, Nikolay Kosinov, Emiel J. M. Hensen
Summary: In this study, Cu-based catalysts were synthesized using different methods, with the addition of CeO2 found to enhance the CH3OH selectivity of Cu/ZnO-CeO2 catalysts. In situ IR spectroscopy revealed insights into the CO2 hydrogenation mechanism over Cu-Zn-Ce oxide catalysts.
Article
Chemistry, Physical
Zeynep Ayla, Darshan Patel, Arzam Harris, David W. Flaherty
Summary: This study found that atomically dispersed Ti sites on metal oxides can activate H2O2 to create intermediates active for alkene epoxidation reactions. By comparing reaction rates, electronic properties, and non-covalent interactions on different metal oxide catalysts, the researchers discovered a correlation between water adsorption at the solid-liquid interface and the stability of epoxidation transition states.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Physical
Christian J. Breckner, Kuixin Zhu, Mingrui Wang, Guanghui Zhang, Christina W. Li, Jeffrey T. Miller
Summary: This study aimed to control the active site coverage of metallic nanoparticles to lower levels than previous SMSI catalysts, in order to improve the reaction rate while maintaining high selectivity. The results showed that the Ti loading and reduction temperature played important roles in determining the SMSI coverage.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Zhiyuan Wang, Yinjian Zheng, Jiye Feng, Wenbiao Zhang, Qingsheng Gao
Summary: Pd/MoO3-x catalysts were proposed for the reductive amination of furfural, showing high catalytic activity due to the interactions between Pd nanoparticles and MoO3-x supports. The Mo-V-rich MoO3-x acts as an acidic promoter to facilitate carbonyl group activation and also interacts with Pd nanoparticles to promote hydrogenolysis reactions. The efficient Pd/MoO3-x catalyst demonstrates the importance of metal-support interactions in biomass refinery.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Yinjian Zheng, Zhiyuan Wang, Peng Chen, Wenbiao Zhang, Qingsheng Gao
Summary: The electro-reductive coupling of nitro and carbonyl compounds provides a convenient, environmentally friendly and energy benign method for the synthesis of valuable nitrones or imines, but achieving high selectivity remains challenging. In this study, the surface roughness of Cu electrodes is introduced as a determinant to control the switch from nitrones to imines by the controllable reduction of nitroarenes on tailored Cu-I/Cu-0 interfaces. The selectivity of nitrones and imines can be modulated by adjusting the roughness of the Cu electrode, with higher roughness leading to decreased nitrones and increased imines. This surface roughness-dependent selectivity is demonstrated in a wide range of substrates, highlighting the potential of surface engineering for electrochemical synthesis.
Article
Engineering, Chemical
Fei Yuan, Guanghui Zhang, Mingrui Wang, Jie Zhu, Miao Zhang, Fanshu Ding, Zening Cheng, Chunshan Song, Xinwen Guo
Summary: This study reports a series of Fe-Co bimetallic catalysts derived from Fe-Co-Mg layered double hydroxides (LDHs) with different Fe/Co ratios for converting CO2 to light olefins. The best catalyst, FeCo-9:1-LDH, showed a high selectivity of C-2-C-4(=) over 36% at a CO2 conversion higher than 40%. The catalyst can be carburized to Co-modified iron carbide (Fe5C2), which exhibits higher CO2 conversion and C-2-C-4(=) selectivity compared to the catalyst prepared by impregnating Co and Fe onto MgO support.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Physical
Bin Zhao, Xiaoqiang Zhang, Jingbo Mao, Yanli Wang, Guanghui Zhang, Zongchao Conrad Zhang, Xinwen Guo
Summary: This study investigates the effect of different crystalline surfaces of TiO2 on the activity of Au-supported catalysts during the hydrodeoxygenation process. It is found that the easy reduction of the TiO2-101 surface and the formation of Aud- promote the demethylation of guaiacol, leading to high activity of Au/TiO2-101 catalyst. On the other hand, the lower activity of Au/TiO2-001 catalyst is attributed to the difficulty in reducing the TiO2-001 surface and the absence of Aud-.
Article
Multidisciplinary Sciences
Mingrui Wang, Peng Wang, Guanghui Zhang, Zening Cheng, Mengmeng Zhang, Yulong Liu, Rongtan Li, Jie Zhu, Jianyang Wang, Kai Bian, Yi Liu, Fanshu Ding, Thomas P. Senftle, Xiaowa Nie, Qiang Fu, Chunshan Song, Xinwen Guo
Summary: In this study, an in situ synthesized K-Co2C catalyst was developed for CO2 hydrogenation, achieving a selectivity of 67.3% for C2+ hydrocarbons. Experimental and theoretical results showed that CoO transformed into Co2C, and the stability of Co2C depended on the reaction atmosphere and the K promoter. The formation of surface C* species was facilitated by the co-action of K promoter and H2O, while the adsorption of C* on CoO was enhanced by the K promoter. The addition of H2O extended the lifetime of K-Co2C from 35 hours to over 200 hours.
Review
Chemistry, Multidisciplinary
Wanling Zhang, Wenbiao Zhang, Jingwen Tan, Yi Tang, Qingsheng Gao
Summary: This review provides an overview of Chevrel phases (CPs) with the chemical formula of MxMo6T8 (T = S, Se, and Te) as noble-metal-free electrocatalysts. It focuses on the representative efforts made and progress achieved in exploring the crystal structure and surface configurations to enhance efficiency. The design, fabrication, and catalytic performance of CPs are discussed in detail, and the potential of CPs in electrocatalysis is highlighted. The review aims to deepen the understanding of CPs and inspire the development of more cost-efficient catalysts.
MATERIALS CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Multidisciplinary
Yinqiong Wu, Jiye Feng, Danni Shi, Wenbiao Zhang, Yi Tang, Qingsheng Gao
Summary: Hierarchical Cu dendrites fabricated via Cl-mediated electrodeposition exhibit high C2H4 efficiency (58% faradaic efficiency at -0.9 V vs. RHE) for CO2 electroreduction due to their optimal hydrophobicity/aerophilicity and dominant distribution of active (100) and (110) facets.
CHEMICAL COMMUNICATIONS
(2023)
Review
Chemistry, Physical
Jingwen Tan, Mei Jiang, Kun Yu, Yuyang Song, Wenbiao Zhang, Qingsheng Gao
Summary: The electrochemical upgradation of biomass feedstock is important for achieving carbon cycle without high-grade heat sources. Notably, Cu-based catalysts enable efficient and selective conversion of furanic molecules through electrochemical hydrogenation and oxidation. This review provides insights into the electrochemical processes and discusses the achievements in catalytic performance, mechanism, and electronic efficiency improvement. Future developments in electrocatalysts and electrolysis techniques are also anticipated.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Brandon C. C. Bukowski, Stephen C. C. Purdy, Evan C. C. Wegener, Zhenwei Wu, A. Jeremy Kropf, Guanghui Zhang, Jeffrey T. T. Miller, Jeffrey Greeley
Summary: Synchrotron spectroscopy and Density Functional Theory (DFT) are combined to develop a new descriptor for the stability of adsorbed chemical intermediates on metal alloy surfaces. The descriptor is related to shifts in Resonant Inelastic X-ray Scattering (RIXS) signals and provides a connection to traditional descriptions of chemisorption. The accessibility of this descriptor to both DFT calculations and experimental spectroscopy allows for deeper connections between theory and characterization in the discovery of new catalysts.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Wenbiao Zhang, Wanling Zhang, Jingwen Tan, Di Pan, Yi Tang, Qingsheng Gao
Summary: This study demonstrates the use of two-dimensional Pd-based metallenes as efficient electrocatalysts for the electrocatalytic hydrogenation of nitroarenes, showing the intrinsic promotion of active sites by alloying effects. Among them, a Pd-Mo metallene with a highly exposed active surface and strong electronic interactions between Pd and Mo atoms exhibits high selectivity (>90.0%) and faradaic efficiency (78.3%) for the chemoselective hydrogenation of 4-nitrostyrene (4-NS) to value-added 4-vinylaniline (4-VA), outperforming a homemade Pd metallene and commercial Pd/C.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Mei Jiang, Jingwen Tan, Yizhong Chen, Wenbiao Zhang, Peng Chen, Yi Tang, Qingsheng Gao
Summary: The promoted electrocatalytic hydrogenation of biomass-derived furfural to 2-methylfuran is identified for the first time in a water/oil bi-phasic system, with the oil phase enabling rapid separation of hydrophobic products from the electrode/electrolyte interfaces, leading to a favorable equilibrium for hydrodeoxygenation.
CHEMICAL COMMUNICATIONS
(2023)
Article
Nanoscience & Nanotechnology
Boxu Gao, Xue Yang, Xueliang Fan, Zhuxin Gui, Wenbiao Zhang, Yingshuai Jia, Sinong Wang, Yahong Zhang, Qingsheng Gao, Yi Tang
Summary: In this research, a three-step preactivation process was proposed to reconstruct commercial nickel foam (CNF) as an efficient electrocatalyst for the oxygen evolution reaction (OER). The activated CNF showed excellent OER performance in alkaline media and could tolerate long-term tests under a large current density. The calcination step led to a reconstructive surface morphology, the high-voltage treatment changed the valence of surface Ni species, and the immersion process introduced Fe heteroatoms into the CNF surface, all contributing to the improved catalytic performance.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Wanjun Ou, Wenbiao Zhang, Haoran Qin, Weijia Zhou, Yi Tang, Qingsheng Gao
Summary: Introducing Mo-doping enhances the electrocatalytic activity and anti-chlorine corrosion properties of Ni3S2, leading to efficient overall seawater splitting.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2024)
Article
Chemistry, Physical
Rui Gao, Zhongyu Qiu, Kun Xu, Zihui Zhai, Yuanyuan Cong, Qike Jiang, Guanghui Zhang, Yang Lv, Yizheng Guo, Yongpeng Li, Qingchuan Xu, Yi Xiao, Yiheng Pang, Yun Wang, Yujiang Song
Summary: In this study, F-decorated Fe-N-C was synthesized by pyrolysis of trifluoromethyl imidazole decorated zeolitic imidazolate framework-8 with hemin as Fe precursor. F-Fe-N-C exhibits exceptional activity with high half-wave potential and single cell power density. The enhancement in performance is attributed to the high activity of F-Fe-N-C, abundant pore volume, and scattered distribution of ionomer.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)