Article
Chemistry, Multidisciplinary
Xiaoyi Zhang, Liying Xiao, Zhaozhao Ding, Qiang Lu, David L. Kaplan
Summary: Beta-sheet rich silk nanofiber hydrogels with improved mechanical properties were successfully prepared by actively regulating the assembly of silk nanofibers through insights into their structure. The resulting hydrogels exhibited superior modulus, ultimate stress, and toughness compared to previous silk hydrogels. The dense gel network and high beta-sheet content of these hydrogels provided stability and anti-swelling ability. Furthermore, the modulus of the hydrogels could be modulated to provide differentiation signals to stem cells. This study highlights the importance of understanding silk nanofibers for developing high-performance biomaterials.
Article
Biochemistry & Molecular Biology
Aisha Fahim, Onofrio Annunziata
Summary: The addition of small amounts of HEPES near physiological ionic strength is essential for converting protein-rich droplets into compact tetragonal crystalline microparticles, which exhibit small size, narrow size distribution, and guest-binding properties. The interactions between lysozyme and HEPES were found to be weakly attractive and exothermic. These findings suggest that salting-in type additives play an important role in controlling the fate of metastable protein-rich microdroplets.
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
(2021)
Article
Chemistry, Multidisciplinary
Dillan Stengel, J. Bennett Addison, David Onofrei, Nha Uyen Huynh, George Youssef, Gregory P. Holland
Summary: This study revealed the unique water-induced cross-linking mechanism in orb-weaving spider aciniform silk, increasing the beta-sheet content and stiffness of the silk. Mechanical shear further enhances beta-sheet cross-linking, resulting in 4-6 nm beta-sheet domains. The observation of converting a flexible alpha-helix-rich fiber to a rigid beta-sheet mat through water treatment may open new possibilities in bioinspired materials design.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Thermodynamics
Ondrej Hajek, Milan Maly, Jan Jedelsky, Sai Krishna Vankeswaram, Ondrej Cejpek, Frantisek Prinz, Miroslav Jicha
Summary: This paper focuses on the dispersion of a liquid jet impacting on a single stainless steel rod studied with high-speed visualization. Two liquid sheets are formed, and the dispersion angle and breakup length are related to the liquid flow rate and orifice diameter. Multiple breakup regimes are observed in the recorded images, depending on the impact velocity.
EXPERIMENTAL THERMAL AND FLUID SCIENCE
(2023)
Article
Nanoscience & Nanotechnology
Emma Olson, Justin S. Plaut, Sarah A. Barnhill, Sinan Sabuncu, Corey M. Dambacher, Sean D. Speese, Srivathsan Ranganathan, Bruce P. Branchaud, Adem Yildirim
Summary: A sensitive method for detecting protease activity using a beta-sheet-rich nanoplatelet-forming peptide precursor and thioflavin T has been developed, allowing for detection of specific proteases like legumain. This method shows promise for various protease-detection applications due to its simplicity and low cost, and does not require time-consuming conjugation reactions or purification steps.
ACS APPLIED NANO MATERIALS
(2021)
Article
Multidisciplinary Sciences
Taylor J. B. Forrester, Olga G. Ovchinnikova, Zhixiong Li, Elena N. Kitova, Jeremy T. Nothof, Akihiko Koizumi, John S. Klassen, Todd L. Lowary, Chris Whitfield, Matthew S. Kimber
Summary: WbbB, a structurally unusual retaining glycosyltransferase, forms an Asp232-Kdo adduct prior to transfer. This double-displacement mechanism, first proposed in 1953, differs from other glycosyltransferases. Structural analysis shows that WbbB repositions the Kdo into a second sub-site for transfer. The study suggests that retaining glycosyltransferases can use double-displacement mechanisms.
NATURE COMMUNICATIONS
(2022)
Article
Engineering, Chemical
Ruizhuan Wang, Guzhong Chen, Hao Qin, Hongye Cheng, Lifang Chen, Zhiwen Qi
Summary: Screening bifunctional ionic liquids can enhance the efficiency of long-chain ester formation, with evaluation of extraction and catalytic performance based on infinite dilution selectivity and pKa values. Experimental results show that the screened IL outperforms commonly used bifunctional IL in terms of long-chain ester yield and purity.
CHEMICAL ENGINEERING SCIENCE
(2021)
Article
Engineering, Environmental
Guokai Cui, Yisha Xu, Daqing Hu, Ying Zhou, Chunliang Ge, Huayan Liu, Wenyang Fan, Zekai Zhang, Biao Chen, Quanli Ke, Yaoji Chen, Bing Zhou, Wei Zhang, Ruina Zhang, Hanfeng Lu
Summary: A series of functional ionic deep eutectic solvents (iDESs) containing pyridinolate anions were developed as green sorbents, solvents, and catalysts for the efficient capture and transformation of CO2 to quinazoline-2,4 (1H,3H)-dione and its derivatives. The physical properties of the iDESs were investigated, and the effects of CO2 partial pressure and absorption temperature on CO2 absorption capacity were studied. The CO2 absorption mechanism and reaction thermodynamics were analyzed, and the effects of various factors on CO2 conversion were systematically studied.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Engineering, Environmental
Man Zhang, Rubo Tian, Siyang Tang, Kejing Wu, Binshen Wang, Yingying Liu, Yingming Zhu, Houfang Lu, Bin Liang
Summary: Bamboo powder waste from bamboo pulp and papermaking can be effectively separated using an integrated approach involving mechanical activation, hydrothermal extraction, and deep eutectic solvents (DESs) delignification. Choline chloride (ChCl)-lactic acid (La) DES (1:1) is the most efficient in lignin removal (78.0%) while retaining cellulose (88.9%). The delignification rate is negatively correlated with carboxyl group amount and higher for DESs with lower pKa values. DES treatment degrades guaiacyl unit lignin fractions and disrupts 8-arylether bonds. DESs exhibit good recyclability with less than 10% reduction in delignification after three cycles. The study demonstrates the practical significance of multistage treatment for biomass fractionation.
Article
Chemistry, Physical
Snehashis Nandi, Luis Padrela, Lidia Tajber, Alain Collas
Summary: The fundamental understanding of solubility and nucleation kinetics is crucial for the development of liquid antisolvent crystallization (LASC) process. This study determined the solubility of intermediate A in different solvents and binary mixtures using a liquid chromatographic method. The selection of the optimum scale and mixing conditions for measuring the metastable zone width (MSZW) in nucleation kinetics was demonstrated to be important. The derived kinetic parameters and accurate solubility data can guide solvent selection for the generation of nanosuspensions in LASC.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Chemistry, Analytical
Xiaochong Song, Siyu Luo, Jun Liu, Yuanfei Wu, Xiaojia Huang
Summary: Efficient separation and enrichment of Se(iv) and Se(vi) species in water samples were achieved in this study using online monolith-based magnetic field-assisted in-tube solid phase microextraction (MFA/IT-SPME). The application of a magnetic field during the extraction procedure significantly improved the extraction efficiency. The developed method combined with HPLC allowed for the quantification of Se(iv) and Se(vi) in environmental water samples with satisfactory results.
Article
Engineering, Chemical
Shaoxiao Liu, Fangyuan Yang, Jin Zhou, Yu Peng, Enlin Wang, Junjie Song, Baowei Su
Summary: In this study, a new type of thin film composite (TFC) membrane with high selective permeability for organic solvent nanofiltration (OSN) was successfully fabricated using low concentrations of MPD and β-CD. It was found that the addition of β-CD could improve the hydrophilicity and pore size of the membrane. The optimized OSN membrane exhibited excellent solvent resistance and catalyst recovery performance.
JOURNAL OF MEMBRANE SCIENCE
(2023)
Article
Electrochemistry
Yu Wu, Qintao Sun, Yue Liu, Peiping Yu, Bingyun Ma, Hao Yang, Miao Xie, Tao Cheng
Summary: Metallic lithium is a promising material for rechargeable lithium-based batteries, but its application is hindered by the growth of lithium dendrites and the formation of dead lithium. A recent electrolyte, with low concentration and containing a single salt and two solvents, has attracted attention due to its ability to achieve high energy efficiency. However, the underlying reaction mechanism and structure of the solid electrolyte interface (SEI) are still unclear, which poses challenges for further improvement. By using a hybrid ab initio and reactive force field (HAIR) method, the authors of this study revealed the reaction mechanisms and formation pathway of the SEI. Their findings provide valuable insights for the design of advanced electrolytes.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Applied
Melasinee Laosuwan, Choosak Poonsawat, Rodjana Burakham, Supalax Srijaranai, Siriboon Mukdasai
Summary: A novel liquid colorimetric sensor based on deep eutectic solvent (DES) was developed for preconcentration and detection of Pb2+ in various food samples, showing advantages of simplicity, rapidity, environmental friendliness, and low cost.
Article
Engineering, Environmental
Qiuju Li, Xueyu Wang, Lianjun Song, Lanlan He, Qiao Yu, Xiao Xiao, Songdong Ding
Summary: In this study, it was found that by introducing cyclohexyl substituent to the DGA ligand skeleton, the extractability of Sr2+ in HNO3 solution could be significantly enhanced, and the effect is more significant with more cyclohexyl substituents.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2023)
Article
Engineering, Biomedical
Peter A. Johnson, Sara Menegatti, Adam C. Chambers, Dominic Alibhai, Tracey J. Collard, Ann C. Williams, Hagan Bayley, Adam W. Perriman
Summary: This study describes the development of a high-throughput bioprinted colorectal cancer (CRC) spheroid platform that is highly automated and provides rich information content, with low cell number requirement. By using a hydrogel bioink with a compressive Young's modulus similar to that of colonic tissue, spheroids from various CRC cell lines can grow exponentially. The study also found that bioprinted CRC spheroids exhibit higher levels of chemoresistance compared to cell monolayers.
Review
Chemistry, Multidisciplinary
Ning Gao, Stephen Mann
Summary: Complex coacervate microdroplets derived from associative phase separation have shown great potential in constructing membraneless protocells. However, the lack of an enclosing membrane limits their functionality. In this Account, we present chemical strategies for the membranization of coacervate microdroplets and discuss their potential applications as functional materials. We hope that this Account will inspire further research and development in this field.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Review
Chemistry, Multidisciplinary
Charles de Kergariou, Frederic Demoly, Adam Perriman, Antoine Le Duigou, Fabrizio Scarpa
Summary: 4D printing technology enables the rapid development of multifunctional structures by combining smart materials, stimuli, and additive manufacturing. Hygromorphs, a type of smart material, exhibit properties and morphing capabilities that are dependent on humidity. However, a comprehensive design process for producing hygromorphs using multiple 4D printing techniques is currently unavailable.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Biophysics
Jennifer C. Brookes, Eleanor R. Gray, Colleen N. Loynachan, Michelle J. Gut, Benjamin S. Miller, Alex P. S. Brogan, Rachel A. McKendry
Summary: Protein-protein interactions are crucial for life processes. This study used qualitative and quantitative experimental and computational approaches to investigate the contribution of entropy and enthalpy in nanobodies binding to HIV-1 capsid protein p24. The results showed that differences in entropy between amino acids and water molecules can cause orders of magnitude differences in affinity.
BIOPHYSICAL JOURNAL
(2023)
Article
Materials Science, Multidisciplinary
Charles de Kergariou, Antoine Le Duigou, Adam Perriman, Fabrizio Scarpa
Summary: This work explores the design space of bio-based and humidity-triggered 4D printed shape-changing biocomposites through fabrication, modelling, and testing. The aim is to enhance the understanding of control actuation through printing path tailoring and unlock new applications for biomaterials and autonomous actuator design. The composites, made of flax yarns and polylactic acid matrix filaments, demonstrate moisture-induced actuation. Different composite architectures, including cross-ply configurations, are developed to achieve the desired actuation curvature. A finite element model is used to capture the complexity of the printed hygromorphs.
MATERIALS & DESIGN
(2023)
Article
Chemistry, Multidisciplinary
Omar Rifaie-Graham, Jonathan Yeow, Adrian Najer, Richard Wang, Rujie Sun, Kun Zhou, Tristan N. Dell, Christopher Adrianus, Chalaisorn Thanapongpibul, Mohamed Chami, Stephen Mann, Javier Read de Alaniz, Molly M. Stevens
Summary: This study describes a non-equilibrium nanosystem that utilizes light-gated chemical communication, controllable feedback, and macroscopic oscillations. The system allows for communication between nanoreactors and induces chemical mechanical oscillations in a hydrogel using feedback loops.
Article
Chemistry, Multidisciplinary
Ali Heidari, Oya I. I. Sentuerk, Shuo Yang, Alex Joesaar, Pierangelo Gobbo, Stephen Mann, Tom F. A. de Greef, Seraphine V. V. Wegner
Summary: The authors developed a method to control the communication between sender-receiver pairs in a synthetic cell community through red and blue light illumination. They used photoswitchable membrane adhesion to self-assemble sender and receiver cells into different multicellular structures under red and blue light, allowing specific communication without interference. This work demonstrates the potential for designing orthogonal chemical communication networks in diverse synthetic cell communities.
Article
Chemistry, Multidisciplinary
Hannah Taylor, Ning Gao, Stephen Mann
Summary: We fabricate Janus-like calcium alginate hydrogel microspheres with spatially segregated populations using microfluidics. These microspheres serve as integrated platforms for domain-mediated chemical communication and programmable protocell-matrix dynamics. Our results offer new possibilities for the design and construction of spatially organized cytomimetic consortia capable of endogenous chemical processing and protocell-environment interactivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemistry & Molecular Biology
Thomas R. Harrison, Vijai Kumar Gupta, Parvez Alam, Adam Willis Perriman, Fabrizio Scarpa, Vijay Kumar Thakur
Summary: The recognition of the harm caused by conventional and fossil-based materials, particularly single-use and non-biodegradable plastics, is increasing. Therefore, addressing climate change and plastic waste pollution requires a more responsible approach to sourcing raw materials and using less destructive end-of-life pathways. This review assesses recent studies on manure-based cellulose materials, examining their material characteristics and implications for sustainability.
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
(2023)
Article
Chemistry, Multidisciplinary
Yanwen Zhang, Zefeng Wang, Mei Li, Can Xu, Ning Gao, Zhuping Yin, Kemin Wang, Stephen Mann, Jianbo Liu
Summary: The design and construction of synthetic protocells capable of stimuli response and homeostatic regulation is an important challenge for synthetic protobiology. In this study, we demonstrate a reconfigurable model protocell based on osmotic reconfiguration of lipid-coated coacervate droplets into multicompartmentalized coacervate vesicles that can exhibit hypotonic stress-induced volume response and enhance enzyme reactions. The increased nitric oxide (NO) within the swollen vesicles can induce blood vessel vasodilation, showing potential applications in biomedicine, cellular diagnostics, and bioengineering.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Review
Chemistry, Multidisciplinary
Chengying Yin, Xingyu Jiang, Stephen Mann, Liangfei Tian, Bruce W. Drinkwater
Summary: The high throughput deposition of microscale objects with precise spatial arrangement is crucial in microfabrication technology. The utilization of dynamic acoustic fields offers a contactless approach to real-time reconfigurable miniaturized systems, with potential applications in various fields. This article discusses the physical interactions of microscale objects in an acoustic pressure field, the fabrication of acoustic trapping devices, methods to tune the spatial arrangement, and potential applications in different disciplines.
Article
Multidisciplinary Sciences
Zhijun Xu, Jiarui Qi, Shengliang Wang, Xiaoman Liu, Mei Li, Stephen Mann, Xin Huang
Summary: The researchers achieved sustainable hydrogen production for over 200 days by coating algal cells with an ultra-thin Fe(III)-doped polypyrrole inner layer and an outer exoskeleton of CaCO3. This cellular bionic approach enhances green hydrogen production under environmentally benign conditions.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Patrick J. Grimes, Mary Jenkinson-Finch, Henry E. Symons, Wuge H. Briscoe, Sebastien Rochat, Stephen Mann, Pierangelo Gobbo
Summary: The synthesis of a novel photocleavable, poly(ethylene) glycol-based crosslinker enables the realization of light-induced disassembly, pattern generation and membrane permeability modulation in protocells, opening up new avenues for the engineering of organized protocell networks and micro-compartmentalized systems for information storage and release.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Zhuping Yin, Ning Gao, Can Xu, Mei Li, Stephen Mann
Summary: This article describes a self-driven, endosymbiotic-like pathway where proteinosomes are captured within membranized alginate/silk fibroin coacervate vesicles by guest-mediated reconfiguration. The interchange of coacervate vesicle and droplet morphologies through proteinosome-mediated activity produces discrete nested communities with integrated catalytic activity and selective disintegration.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Review
Materials Science, Biomaterials
Naomi Akiyama, Kapil D. Patel, Eun Jo Jang, Mark R. Shannon, Rajkumar Patel, Madhumita Patel, Adam Willis Perriman
Summary: The composition, morphology, and mechanical performance of nanomaterials are crucial for tissue engineering. Tubular nanomaterials (TNs), including carbon nanotubes, titanium oxide nanotubes, halloysite nanotubes, silica nanotubes, and hydroxyapatite nanotubes, have shown great potential in various applications due to their high surface area, versatile surface chemistry, well-defined mechanical properties, excellent biocompatibility, and monodispersity. This review focuses on the recent developments in TN-based biomaterials for structural tissue engineering, with a strong emphasis on bone tissue regeneration. It includes a detailed literature review on TN-based orthopedic coatings for metallic implants and composite scaffolds to enhance in vivo bone regeneration.
JOURNAL OF MATERIALS CHEMISTRY B
(2023)
