An optoelectronic material with a spatially varying bandgap that is tunable is highly desirable for use in photovoltaics, photocatalysis and photodetection. Elastic strain has the potential to be ...used to achieve rapid and reversible tuning of the bandgap. However, as a result of plasticity or fracture, conventional materials cannot sustain a high enough elastic strain to create sufficient changes in their physical properties. Recently, an emergent class of materials--named 'ultrastrength materials'--have been shown to avoid inelastic relaxation up to a significant fraction of their ideal strength. Here, we illustrate theoretically and computationally that elastic strain is a viable agent for creating a continuously varying bandgap profile in an initially homogeneous, atomically thin membrane. We propose that a photovoltaic device made from a strain-engineered MoS2 monolayer will capture a broad range of the solar spectrum and concentrate excitons or charge carriers.
Red phosphorus is a promising photocatalyst with wide visible‐light absorption up to 700 nm, but the fast charge recombination limits its photocatalytic hydrogen evolution reaction (HER) activity. ...Now, 001‐oriented Hittorf's phosphorus (HP) nanorods were successfully grown on polymeric carbon nitride (PCN) by a chemical vapor deposition strategy. Compared with the bare PCN and HP, the optimized PCN@HP hybrid exhibited a significantly enhanced photocatalytic activity, with HER rates reaching 33.2 and 17.5 μmol h−1 from pure water under simulated solar light and visible light irradiation, respectively. It was theoretically and experimentally indicated that the strong electronic coupling between PCN and 001‐oriented HP nanorods gave rise to the enhanced visible light absorption and the greatly accelerated photoinduced electron–hole separation and transfer, which benefited the photocatalytic HER performance.
001‐oriented hexagonal‐shaped Hittorf's phosphorus (HP) nanorods with exposed {110} facets were grown on polymeric carbon nitride (PCN) for boosting photocatalytic hydrogen evolution from pure water. The enhanced visible light absorption and accelerated charge transfer efficiency through the P−N bonds and the 001‐oriented HP nanorods were crucial for the improved photocatalytic activity.
Fuel cells are considered as a promising alternative to the existing traditional energy systems towards a sustainable future. Nevertheless, the synthesis of efficient and robust platinum (Pt) based ...catalysts remains a challenge for practical applications. In this work, we present a simple and scalable molten‐salt synthesis method for producing a low‐platinum (Pt) nanoalloy implanted in metal–nitrogen–graphene. The as‐prepared low‐Pt alloyed graphene exhibits a high oxygen reduction activity of 1.29 A mgPt−1 and excellent durability over 30 000 potential cycles. The catalyst nanoarchitecture of graphene encased Pt nanoalloy provides a robust capability against nanoparticle migration and corrosion due to a strong metal–support interaction. Similarly, advanced characterization and theoretical calculations show that the multiple active sites in platinum alloyed graphene synergistically account for the improved oxygen reduction. This work not only provides an efficient and robust low‐Pt catalyst but also a facile design idea and scalable preparation technique for integrated catalysts to achieve more profound applications in fuel cells and beyond.
Pt−Co nanoalloys planted in the metal–nitrogen–graphene system achieved by a scalable molten salt pyrolysis method demonstrate improved activity and stability for oxygen reduction through a synergistic effect among multiple active sites and a strong metal–support interaction.
Rational design and synthesis of hetero‐coordinated moieties at the atomic scale can significantly raise the performance of the catalyst and obtain mechanistic insight into the oxygen‐involving ...electrocatalysis. Here, a facile plasma‐photochemical strategy is applied to construct atomically coordinated Pt–Co–Se moieties in defective CoSe2 (CoSe2−x) through filling the plasma‐created Se vacancies in CoSe2−x with single Pt atomic species (CoSe2−x‐Pt) under ultraviolet irradiation. The filling of single Pt can remarkably enhance the oxygen evolution reaction (OER) activity of CoSe2. Optimal OER specific activity is achieved with a Pt content of 2.25 wt% in CoSe2−x‐Pt, exceeding that of CoSe2−x by a factor of 9. CoSe2−x‐Pt shows much better OER performance than CoSe2−x filled with single Ni and even Ru atomic species (CoSe2−x‐Ni and CoSe2−x‐Ru). Noticeably, it is general that Pt is not a good OER catalyst but Ru is; thus the design of active sites for electrocatalysis at an atomic level should follow a different intrinsic mechanism. Mechanism studies unravel that the single Pt can induce much higher electronic distribution asymmetry degree than both single Ni and Ru, and benefit the interaction between the Co sites and adsorbates (OH*, O*, and OOH*) during the OER process, leading to a better OER activity.
Atomically coordinated Pt–Co–Se moieties are generated by filling Se vacancies in defective CoSe2 with single Pt atoms (CoSe2−x‐Pt) under ultraviolet irradiation. Even though Pt is not a good oxygen evolution reaction (OER) catalyst, single Pt can induce a higher electronic distribution asymmetry degree than single Ni and Ru, and benefit the interaction between Co sites and adsorbates, endowing CoSe2−x‐Pt with much better OER performance.
This research employed a conventional solid-state technique to synthesize a novel AgMoVO
6
ceramic material and conducted an analysis of its microwave dielectric properties. The analysis revealed ...that the sample synthesized at 520 °C possessed a monoclinic structure and belonged to the C2/m (12) space group, indicating a pure AgMoVO
6
phase. The dielectric constant of the ceramic was primarily influenced by its density, porosity, and ionic polarizability. Moreover, an increase in the packing fraction and lattice energy significantly enhanced the
Q
×
f
values of the ceramic. The correlation between the bond valence of the specimen and its
τ
f
value was found to be strong. Furthermore, the study demonstrated that the dielectric characteristics of the specimens were highly dependent on their unit-cell volume, which critically affected their microwave dielectric properties. Notably, the phase-pure AgMoVO
6
ceramic exhibited exceptional dielectric properties at microwave frequencies, with an
ε
r
of ~ 12.4,
Q
×
f
of ~ 21,300 GHz, and
τ
f
of ~ –46.9 ppm/°C. Additionally, the ceramic material has been successfully employed in the design of a dual-band filter, showcasing its potential for utilization in 5G systems.
Ras gene mutation and/or overexpression are drivers in the progression of cancers, including colorectal cancer. Blocking the Ras signaling has become a significant strategy for cancer therapy. ...Previously, we constructed a recombinant scFv, RGD-p21Ras-scFv by linking RGD membrane-penetrating peptide gene with the anti-p21Ras scFv gene. Here, we expressed prokaryotically RGD-p21Ras-scFv on a pilot scale, then investigated the anti-tumor effect and the mechanism of blocking Ras signaling.
The E. coli bacteria which could highly express RGD-p21Ras-scFv was screened and grown in 100 L fermentation tank to produce RGD-p21Ras-scFv on optimized induced expression conditions. The scFv was purified from E. coli bacteria using His Ni-NTA column. ELISA was adopted to test the immunoreactivity of RGD-p21Ras-scFv against p21Ras proteins, and the IC50 of RGD-p21Ras-scFv was analyzed by CCK-8. Immunofluorescence colocalization and pull-down assays were used to determine the localization and binding between RGD-p21Ras-scFv and p21Ras. The interaction forces between RGD-p21Ras-scFv and p21Ras after binding were analyzed by molecular docking, and the stability after binding was determined by molecular dynamics simulations. p21Ras-GTP interaction was detected by Ras pull-down. Changes in the MEK-ERK /PI3K-AKT signaling paths downstream of Ras were detected by WB assays. The anti-tumor activity of RGD-p21Ras-scFv was investigated by nude mouse xenograft models.
The technique of RGD-p21Ras-scFv expression on a pilot scale was established. The wet weight of the harvested bacteria was 31.064 g/L, and 31.6 mg RGD-p21Ras-scFv was obtained from 1 L of bacterial medium. The purity of the recombinant antibody was above 85%, we found that the prepared on a pilot scale RGD-p21Ras-scFv could penetrate the cell membrane of colon cancer cells and bind to p21Ras, then led to reduce of p21Ras-GTP (active p21Ras). The phosphorylation of downstream effectors MEK-ERK /PI3K-AKT was downregulated. In vivo antitumor activity assays showed that the RGD-p21Ras-scFv inhibited the proliferation of colorectal cancer cell lines.
RGD-p21Ras-scFv prokaryotic expressed on pilot-scale could inhibited Ras-driven colorectal cancer growth by partially blocking p21Ras-GTP and might be able to be a hidden therapeutic antibody for treating RAS-driven tumors.
Facile and reliable screening of cost-effective, high-performance and scalable electrocatalysts is key for energy conversion technologies such as water splitting. ABO
perovskites, with rich ...constitutions and structures, have never been designed via activity descriptors for critical hydrogen evolution reaction (HER). Here, we apply coordination rationales to introduce A-site ionic electronegativity (AIE) as an efficient unifying descriptor to predict the HER activities of 13 cobalt-based perovskites. Compared with A-site structural or thermodynamic parameter, AIE endows the HER activity with the best volcano trend. (Gd
La
)BaCo
O
predicted from an AIE value of ~2.33 exceeds the state-of-the-art Pt/C catalyst in electrode activity and stability. X-ray absorption and computational studies reveal that the peak HER activities at a moderate AIE value of ~2.33 can be associated with the optimal electronic states of active B-sites via inductive effect in perovskite structure (~200 nm depth), including Co valence, Co-O bond covalency, band gap and O 2p-band position.
To achieve the most efficiency in supply chain management, the capability of distribution networks is a key point for the entire supply chain. Stocks are critical for enhancing the efficiency of ...satisfying the demand of retailers in the distribution network. A configuration of a distribution network is consisted of routes and nodes. Each route connects a pair of nodes and each node is denoted as a supplier, a distribution center, or a retailer. For each route, it has a carrier whose available capacity for demand transmission is multi state. Hence, a distribution network is also regarded as a multi state network and such a network is named as a multi state distribution network (MDN) in here. The propose of this paper is to evaluate the system reliability which is defined as the probability that the MDN can meet all retailers’ demand under stocks. In practical, all retailers’ demand should be satisfied by stocks in the distribution centers (DCs) firstly. Therefore flow assignment in MDN model is mainly clarified by the relationship between the demand of retailers, stocks on DCs, and suppliers. The concept of minimal capacity vectors (MCVs) is then proposed and an algorithm is developed to obtaining MCVs for evaluating system reliability.
The nitrogenous nucleophile electrooxidation reaction (NOR) plays a vital role in the degradation and transformation of available nitrogen. Focusing on the NOR mediated by the β‐Ni(OH)2 electrode, we ...decipher the transformation mechanism of the nitrogenous nucleophile. For the two‐step NOR, proton‐coupled electron transfer (PCET) is the bridge between electrocatalytic dehydrogenation from β‐Ni(OH)2 to β‐Ni(OH)O, and the spontaneous nucleophile dehydrogenative oxidation reaction. This theory can give a good explanation for hydrazine and primary amine oxidation reactions, but is insufficient for the urea oxidation reaction (UOR). Through operando tracing of bond rupture and formation processes during the UOR, as well as theoretical calculations, we propose a possible UOR mechanism whereby intramolecular coupling of the N−N bond, accompanied by PCET, hydration and rearrangement processes, results in high performance and ca. 100 % N2 selectivity. These discoveries clarify the evolution of nitrogenous molecules during the NOR, and they elucidate fundamental aspects of electrocatalysis involving nitrogen‐containing species.
During urea electrooxidation over a Ni(OH)2 electrode the dehydrogenation reaction from β‐Ni(OH)2 to β‐Ni(OH)O can lead to spontaneous urea dehydrogenation. Spontaneous intramolecular coupling of the N−N bond and hydration of urea dehydrogenation intermediates play important roles in the oxidation path from urea to N2 and CO2.
Plant xylem response to drought is routinely represented by a vulnerability curve (VC). Despite the significance of VCs, the connection between anatomy and tissue‐level hydraulic response to drought ...remains a subject of inquiry. We present a numerical model of water flow in flowering plant xylem that combines current knowledge on diffuse‐porous anatomy and embolism spread to explore this connection. The model produces xylem networks and uses different parameterizations of intervessel connection vulnerability to embolism spread: the Young–Laplace equation and pit membrane stretching. Its purpose is upscaling processes occurring on the microscopic length scales, such as embolism propagation through pit membranes, to obtain tissue‐scale hydraulics. The terminal branch VC of Acer glabrum was successfully reproduced relying only on real observations of xylem tissue anatomy. A sensitivity analysis shows that hydraulic performance and VC shape and location along the water tension axis are heavily dependent on anatomy. The main result is that the linkage between pit‐scale and vessel‐scale anatomical characters, along with xylem network topology, affects VCs significantly. This work underscores the importance of stepping up research related to the three‐dimensional network structure of xylem tissues. The proposed model's versatility makes it an important tool to explore similar future questions.
This work introduces a new open source numerical model of plant xylem. The subject of inquiry is the link between wood anatomy and plant water use, especially vulnerability to embolism under drought. The model successfully reproduces empirical vulnerability curves of Acer terminal branches. The results of this study underscore the importance of stepping up research on the effects of xylem network topology on whole‐plant hydraulics.