Latest ArticlesPt-modified amorphous alloy (Pt@PdNiCuP) catalyst exhibits excellent electro-catalytic activity and high experimental durability for hydrogen evolution reaction (HER). However, the physical origin of the catalytically active remains unclear. In this paper, we constructed a distance contribution descriptor (DCD) for the feature engineering of machine learning (ML) potential, and calculated the Gibbs free energies (ΔGH) of 46,000 *H binding sites on the Pt@PdNiCuP surface by ML-accelerated density functional theory (DFT). The relationship between ΔGH and DCD revealed that in the H-Pt distance region of 2.0–2.5 Å where the parabolic tail and disordered scatters coexist, the H-metal bonding configuration is mainly the bridge- or hollow- bonding type. The contribution analysis of DCD indicates that the joint effect of Pt, Pd and Ni atoms determines the catalytical behavior of amorphous alloy, which agrees well with experimental results. By counting atomic percentages in different energy intervals, we obtained the atomic ratio for the best catalytic performance (Pt:Pd:Ni:Cu:P = 0.33:0.17:0.155:0.16:0.185). Projected density of states (PDOS) show that H 1s orbital, Pt 5d orbital, and Pd 4d orbital form a bonding state at −2 eV. These results provide new ideas for designing more active amorphous alloy catalysts.
Self-immolative linkers have been widely used to construct prodrugs to improve their efficacy and safety. In this study, we report the use of phenoxysilyl linker as a self-immolative unit to prepare antibody-drug conjugates (ADCs). Phenoxysily based ADC Ate-PPS-CA4 was prepared and its release was systematically investigated by mass spectrometry. Biological evaluation showed that Ate-PPS-CA4 displayed the ability to target delivery and self-immolative release the active payload CA4 on PD-L1 positive cells MDA-MB-231. As the same with its payload CA4, it could arrest the cell cycle to the G2/M phase and induced changes in cell morphology at the dose of its IC50. The development of this linker with novel drug release mechanisms will expand the methodology to construct ADCs, especially for non-internalizing ADCs by extracellular cleavage.
In this work, we fabricated an efficient pre-catalyst based on (Ni, Co)S2 solid solution with hierarchical architecture and high porosity to boost urea oxidation reaction and electrocatalytic oxidation of organic small molecules. The interaction between Ni and Co can optimize the electronic structure, resulting in the improved conductivity and accelerated charge transfer rate. The 2D/3D architecture can enrich more active species and endow the mass and electron transport to facilitate the surface oxidation and the following catalytic process. Post-structure and catalytic characterizations confirm the surface oxidation of (Ni, Co)S2 during the stability test, and the in-situ formed Co(Ni) based (oxy)hydroxides exhibit superior catalytic activity and facilitated charge transfer ability. As a result, the optimal (Ni, Co)S2 solid solution pre-catalyst displays facilitated catalytic behavior and good stability for multifunctional electrocatalytic oxidation, in which a high conversion of benzyl alcohol (97.50%), a good selectivity to benzoic acid (93.78%) and a satisfied faraday efficiency (91.86%) can be achieved.
As one of the most promising and practical advanced oxidation processes (AOPs), the catalytic ozonation is triggered by the active components of catalyst, which are usually derived from metals or metal oxides. To avoid the metal pollution from catalyst, here the amorphous boron (A-boron) is used as a metal-free catalyst for catalytic ozonation to produce free radicals for effective degradation of atrazine (ATZ), the world-widely used herbicide and also a widespread pollutant in environment. A-boron exhibits an outstanding performance for catalytic ozonation to remove ATZ from water. As A-boron is introduced into ozonation, the degradation efficiency in 10 min is promoted to 97.1%, much higher than that of 15.1% under ozonation. The mechanism is that the B–B bonds and internal suboxide B in A-boron serve as the main active sites to donate electrons to accelerate ozone decomposition to produce reactive oxygen species (ROS), including •O2− and 1O2, and further enhance ATZ degradation via ROS reactions. Moreover, the A-boron is still highly active with a degradation efficiency of ATZ over 95% in 10 min even after four successive cycles. This work shows A-boron could be an alternative for the active components of metal or metal oxide in catalytic ozonation.
Lanthanide coordinated multicolor fluorescent polymeric hydrogels (MFPHs) are quite promising for various applications because of their sharp fluorescence bands and high color purity. However, few attempts have been carried out to locally regulate their fluorescence switching or shape deforming behaviors, but such studies are very useful for patterned materials with disparate functions. Herein, the picolinate moieties that can sensitize Tb3+/Eu3+ luminescence via antenna effect were chemically introduced into interpenetrating double networks to produce a robust kind of lanthanide coordinated MFPHs. Upon varying the doping ratio of Tb3+/Eu3+, fluorescence colors of the obtained hydrogels were continuously regulated from green to orange and then red. Importantly, spatial fluorescence color control within the hydrogel matrix could be facilely realized by controlled diffusion of Tb3+/Eu3+ ions, producing a number of 2D hydrogel objects with local multicolor fluorescent patterns. Furthermore, the differential swelling capacities between the fluorescent patterned and non-fluorescent parts led to interesting 2D-to-3D shape deformation to give well-defined multicolor fluorescent 3D hydrogel configurations. Based on these results, bio-inspired synergistic color/shape changeable actuators were demonstrated. The present study provided a promising strategy to achieve the local fluorescence and shape control within lanthanide coordinated hydrogels, and is expected to be expanded for fabricating useful patterned materials with disparate functions.
Two-dimensional (2D) layered materials with layer-number dependent properties are promising candidates for next-generation noble-metal-free electrocatalytic reaction. However, the main group metal chalcogenides (MMCs) used for this purpose are rarely explored. Herein, we report the controlled growth of indium selenide (InSe) with a novel morphology (semispherical array) on a silicon substrate and its application in hydrogen evolution reaction (HER). The formation of the spherical InSe is explained with a vapor-liquid-solid growth mechanism, in which the distribution and size of the spheres could be facilely tuned by the reaction parameters. The InSe semispherical array was demonstrated as more efficient catalyst for HER than the flake-like 2D InSe counterparts, originating from the fully exposed InSe spherical surface with abundant adsorbing sites and the high crystalline quality for electron transport. This work provides a controlled synthesis way of the layered InSe with a distinct spherical morphology used for the electrocatalysis applications and could be extended to other main group metal chalcogenides.
We designed a disulfide-crosslinked mini-protein with a two-helical topology consisting of L- and D-amino acids, which was exceptionally stable in serum. Therefore, we further used it as a scaffold to design mini-proteins targeting p53 positive tumor cells. Based on bifunctional grafting, key residues from the transactivation domain of p53 and a designed unnatural amino acid were grafted into the helix constituted by L-amino acids to confer the mini-protein with MDM2 inhibitory activity. Meanwhile, ten Arg residues were introduced to improve its membrane penetrating capacity. Among the mini-proteins, UPROL-10e showed nano-molar binding affinity on MDM2 and cellular toxicity on p53 expressing HCT116 cells.
Defect engineering has been demonstrated to be an appealing strategy to boost the photocatalytic activity of materials. However, can higher defect concentration bring about higher photocatalytic activity? This is an open question. In this work, BiPO4 photocatalysts with controllable oxygen vacancy concentrations were successfully synthesized. The photocatalytic activity of the obtained BiPO4 photocatalysts was determined by the removal of ciprofloxacin and 4-chlorophenol, as well as CO2 photoreduction. The BiPO4 materials with lower oxygen vacancy concentration could display unexpected higher photocatalytic efficiency. Through the investigation of different factors which may affect the photocatalytic performance, such as crystal structure, morphology, specific surface area, defect, and energy band structure, it can be found that the energy band structure difference was responsible for the enhanced photocatalytic activity.
Considering the earth powered by intermittent renewable energy in the coming future, solid oxide electrolysis cell (SOEC) will play an indispensable role in efficient energy conversion and storage on demand. The thermolytic and kinetic merits grant SOEC a bright potential to be directly integrated with electrical grid and downstream chemical synthesis process. Meanwhile, the scientific community are still endeavoring to pursue the SOEC assembled with better materials and operated at a more energy-efficient way. In this review article, at cell level, we focus on the recent development of electrolyte, cathode, anode and buffer layer materials for both steam and CO2 electrolysis. On the other hand, we also discuss the next generation SOEC operated with the assistant of other fuels to further reduce the energy consumption and enhance the productivity of the electrolyzer. And stack level, the sealant, interconnect and stack operation strategies are collectively covered. Finally, the challenges and future research direction in SOECs are included.
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