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1.
Nat Mater ; 21(6): 681-688, 2022 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-35606427

RESUMEN

Atomically dispersed single-atom catalysts have the potential to bridge heterogeneous and homogeneous catalysis. Dozens of single-atom catalysts have been developed, and they exhibit notable catalytic activity and selectivity that are not achievable on metal surfaces. Although promising, there is limited knowledge about the boundaries for the monometallic single-atom phase space, not to mention multimetallic phase spaces. Here, single-atom catalysts based on 37 monometallic elements are synthesized using a dissolution-and-carbonization method, characterized and analysed to build the largest reported library of single-atom catalysts. In conjunction with in situ studies, we uncover unified principles on the oxidation state, coordination number, bond length, coordination element and metal loading of single atoms to guide the design of single-atom catalysts with atomically dispersed atoms anchored on N-doped carbon. We utilize the library to open up complex multimetallic phase spaces for single-atom catalysts and demonstrate that there is no fundamental limit on using single-atom anchor sites as structural units to assemble concentration-complex single-atom catalyst materials with up to 12 different elements. Our work offers a single-atom library spanning from monometallic to concentration-complex multimetallic materials for the rational design of single-atom catalysts.

2.
Langmuir ; 35(50): 16466-16475, 2019 12 17.
Artículo en Inglés | MEDLINE | ID: mdl-31756107

RESUMEN

Site-specific immobilization of proteins on a surface has been a long-lasting challenge in the fields of biosensing and biotechnology because of the need for improving the biological activity of immobilized protein via the maximal exposure of its bioactive domain. Herein, we reported a new site-specific immobilization method for His-tagged proteins onto a vinyl sulfone (VS)-bearing surface in a covalent manner. X-ray photoelectron spectroscopy characterization indicated the specificity of the addition reaction of the imidazole group in histidine on the VS-bearing surface at pH 7.0. Solution-based experiments were carried out to verify the reaction priority of the imidazole residue of histidine with the VS group at neutral conditions. The real-time immobilization process of two His-tagged proteins (HaloTag-6His and anti-HER2 Fab-6His) on surfaces presenting VS, preactivated carboxyl, and NTA groups were studied by quartz crystal microbalance. Compared to the existing methods utilizing covalent (NHS/EDC activated carboxyl) and coordinate (Ni2+-NTA) linking, our method offers two significant advantages for protein immobilization: high density and high specificity. The orientation of the two His-tagged proteins on the VS-bearing surface was confirmed by an enzyme-linked assay and an HER2+ liposome binding experiment. Our method of site-specific immobilization of His-tagged proteins is efficient and straightforward, which would be helpful to expand the applications of recombinant proteins in enzyme immobilization, biosensor and array fabrication, and drug delivery system.


Asunto(s)
Histidina/química , Imidazoles/química , Proteínas Inmovilizadas/química , Sulfonas/química , Adsorción , Modelos Moleculares , Conformación Proteica , Propiedades de Superficie
4.
Environ Pollut ; 257: 113582, 2020 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-31753640

RESUMEN

Dangerous goods are particularly hazardous, as they can be flammable, explosive, and toxic. These characteristics make them vulnerable to accidents, and such mishaps during port operations can lead to massive economic losses and even deaths. It is, therefore, necessary and important to analyze and study the dangerous goods accidents at ports, so as to identify major factors and prevent them. Formal concept analysis (FCA) is a powerful tool for rule extraction. This paper introduces FCA along with relevant documents and case studies to analyze the dangerous goods accidents at China's ports, building a concept lattice model of dangerous goods accidents at China's ports, and reduces the condition attributes to come up with three key attributes of dangerous goods accidents at China's ports: warehousing management, facilities and equipment, goods registration and extract four effective diagnostic rules for dangerous goods accidents at ports. This paper proposes corresponding governance strategies to the rules of dangerous goods accidents, which can significantly prevent and manage dangerous goods accidents at China's ports in the future. In the future, the concept scale can be introduced to study the problem that the influencing factor is multi-valued attribute so as to expand the scope of research.


Asunto(s)
Liberación de Peligros Químicos , Modelos Teóricos , Navíos , Accidentes , China , Predicción
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