Commercial nitric acid (HNO
) and ammonia (NH
) are mostly produced through the Ostwald process and the Haber-Bosch process, respectively. However, high energy demand and enormous greenhouse gas ...accompy these processes. The development of economical and green ways to synthesize HNO
and NH
is highly desirable for solving the global energy and environmental crisis. Here, we present two energy-efficient and environmentally friendly strategies to synthesize HNO
and NH
at distributed sources, including the electrocatalytic oxidation of N
in air to HNO
and the electrocatalytic reduction of residual Formula: see text contamination in water to NH
. The isotope-labeling studies combined with theoretical calculation reveal the reaction path of the two proposed strategies, confirming the origin of the electrochemical products. Importantly, the electrooxidation-generated Formula: see text ions may also serve as reactants for the electroreduction synthesis of NH
in the future. Our work may open avenues for energy-efficient and green production of HNO
and NH
at distributed sources.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
Co‐based metal–organic frameworks (MOFs) as electrocatalysts for two‐electron oxygen reduction reaction (2e− ORR) are highly promising for H2O2 production, but suffer from the intrinsic ...activity‐selectivity trade‐off. Herein, we report a ZnCo bimetal‐triazole framework (ZnCo‐MTF) as high‐efficiency 2e− ORR electrocatalysts. The experimental and theoretical results demonstrate that the coordination between 1,2,3‐triazole and Co increases the antibonding‐orbital occupancy on the Co−N bond, promoting the activation of Co center. Besides, the adjacent Zn−Co sites on 1,2,3‐triazole enable an asymmetric “side‐on” adsorption mode of O2, favoring the reduction of O2 molecules and desorption of OOH* intermediate. By virtue of the unique ligand effect, the ZnCo‐MTF exhibits a 2e− ORR selectivity of ≈100 %, onset potential of 0.614 V and H2O2 production rate of 5.55 mol gcat−1 h−1, superior to the state‐of‐the‐art zeolite imidazole frameworks. Our work paves the way for the design of 2e− ORR electrocatalysts with desirable coordination and electronic structure.
A ZnCo bimetal‐triazole framework has been developed as high‐efficiency 2e− ORR electrocatalysts. The unique ligand effect of 1,2,3‐triazole optimizes the electronic structure of Co sites and enables an asymmetric “side‐on” adsorption mode of O2 molecule, resulting in an excellent 2e− ORR performance with a selectivity of ≈100 % and an H2O2 production rate of 5.55 mol gcat−1 h−1.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
•We employed DEA, Malmquist Index, and Tobit model.•Tech and management are crucial for semiconductor industry growth.•Economic development and R&D investment impact semiconductor industry ...growth.•Intelligent manufacturing methods are worth adopting in the semiconductor industry.
Semiconductors are the cornerstone of rapid information flow in the circular economy era and are crucial for society as a whole. Improving the efficiency and achieving sustainable development of the semiconductor industry are important topics. This research applies the DEA method to evaluate the development efficiency of 36 top semiconductor companies from 2018 to 2022 and together with Malmquist productivity index (MPI) analysis examines the dynamic changes in their efficiency values. We use the Tobit model for regression analysis to determine the impact of four different factors on the sustainable development of the semiconductor industry. The findings are as follows. 1) Insufficient technological capabilities and management experience are the main obstacles to the development of the semiconductor industry, and intelligent manufacturing production methods and technological changes can help this industry achieve transformation and upgrading. 2) Most semiconductor companies have not reached an optimal production scale and can improve themselves by adjusting resource input and production scale. 3) Different regions’ economic development levels and R&D funding play a crucial role in local semiconductor industry development, while trade openness and ecological environment performance also have significant impacts. Finally, we provide targeted recommendations and measures for global semiconductor industry development.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Although clinical studies have shown promise for targeting programmed cell death protein-1 (PD-1) and ligand (PD-L1) signaling in non-small cell lung cancer (NSCLC), the factors that predict which ...subtype patients will be responsive to checkpoint blockade are not fully understood.
We performed an integrated analysis on the multiple-dimensional data types including genomic, transcriptomic, proteomic, and clinical data from cohorts of lung adenocarcinoma public (discovery set) and internal (validation set) database and immunotherapeutic patients. Gene set enrichment analysis (GSEA) was used to determine potentially relevant gene expression signatures between specific subgroups.
We observed that
mutation significantly increased expression of immune checkpoints and activated T-effector and interferon-γ signature. More importantly, the
comutated subgroup manifested exclusive increased expression of PD-L1 and a highest proportion of
Meanwhile,
or
-mutated tumors showed prominently increased mutation burden and specifically enriched in the transversion-high (TH) cohort. Further analysis focused on the potential molecular mechanism revealed that
or
mutation altered a group of genes involved in cell-cycle regulating, DNA replication and damage repair. Finally, immunotherapeutic analysis from public clinical trial and prospective observation in our center were further confirmed that
or
mutation patients, especially those with co-occurring
mutations, showed remarkable clinical benefit to PD-1 inhibitors.
This work provides evidence that
and
mutation in lung adenocarcinoma may be served as a pair of potential predictive factors in guiding anti-PD-1/PD-L1 immunotherapy.
.
Directed energy deposition (DED) is an important additive manufacturing method for producing or repairing high-end and high-value equipment. Meanwhile, the lack of reliable and uniform qualities is a ...key problem in DED applications. With the development of sensing devices and control systems, in situ monitoring (IM) and adaptive control (IMAC) technology is an effective method to enhance the reliability and repeatability of DED. In this paper, we review current IM technologies in IMAC for metal DED. First, this paper describes the important sensing signals and equipment to exhibit the research status in detail. Meanwhile, common problems that arise when gathering these signals and resolvent methods are presented. Second, process signatures obtained from sensing signals and transfer approaches from sensing signals for processing signatures are shown. Third, this work reviews the developments of the IM of product qualities and illustrates ways to realize quality monitoring. Lastly, this paper specifies the main existing problems and future research of IM in metal DED.
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DOBA, EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, IZUM, KILJ, KISLJ, MFDPS, NLZOH, NUK, OBVAL, OILJ, PILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, SIK, UILJ, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
The transport coefficients, in particular the transference number, of electrolyte solutions are important design parameters for electrochemical energy storage devices. The recent observation of ...negative transference numbers in PEO–LiTFSI under certain conditions has generated much discussion about its molecular origins, by both experimental and theoretical means. However, one overlooked factor in these efforts is the importance of the reference frame (RF). This creates a non-negligible gap when comparing experiment and simulation because the fluxes in the experimental measurements of transport coefficients and in the linear response theory used in the molecular dynamics simulation are defined in different RFs. In this work, we show that, by applying a proper RF transformation, a much improved agreement between experimental and simulation results can be achieved. Moreover, it is revealed that the anion mass and the anion–anion correlation, rather than ion aggregates, play a crucial role for the reported negative transference numbers.
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IJS, KILJ, NUK, PNG, UL, UM
Abstract The non-specific interaction between nanoparticles (NPs) and plasma proteins occurs immediately after NPs enter the blood, resulting in the formation of the protein corona that thereafter ...replaces the original NPs and becomes what the organs and cells really see. Consequently, the in vivo fate of NPs and the biological responses to the NPs are changed. This is one substantial reason for the two main problems of the NPs based drug delivery system, i.e. nanotoxicity and rapid clearance of NPs from the blood after intravenous injection. Here, we demonstrate the successful application of the preformed albumin corona in inhibiting the plasma proteins adsorption and decreasing the complement activation, and ultimately in prolonging the blood circulation time and reducing the toxicity of the polymeric PHBHHx NPs. Since the interaction of proteins with various nano-materials and/or -particles is ubiquitous, pre-forming albumin corona has a great potential to be a versatile strategy for optimizing the NPs based drug delivery system.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UL, UM, UPCLJ, UPUK
Defect engineering is an effective way to modulate the electric states and provide active sites for electrocatalytic reactions. However, most studied oxygen vacancies are unstable and susceptible ...under the oxygen circumstance. Here, we fabricated cobalt-defected Co3–x O4 in situ for an efficient oxygen evolution reaction (OER). XAFS and PALS characterizations show that the crystals have abundant Co vacancies and a distorted structure. DFT calculations indicate that the metal defects lead to obvious electronic delocalization, which enhances the carrier transport to participate in water-splitting reactions along the defective conducting channels and the water adsorption/activation on the catalyst surface. Therefore, cobalt-defected Co3–x O4 shows remarkably high OER activity by delivering a much lower overpotential of 268 mV@10 mA cm–2 (with a small Tafel slope of 38.2 mV/dec) for OER in KOH electrolyte, in comparison with normal Co3O4 (376 mV), IrO2 (340 mV), and RuO2 (276 mV). This work opens up a promising approach to construct electronic delocalization structures in metal oxides for high-performance electrochemical catalysts.
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IJS, KILJ, NUK, PNG, UL, UM
Ring-opening reaction via selective cleavage of C-C bond is known as a powerful strategy for construction of complex molecules. Complementary to the ionic process focusing on mostly small ring ...systems, radical-mediated C-C bond cleavage offers a solution for further diverse enantioselective functionalization benefited from its mild conditions, whereas such asymmetric transformations are still limited to three-membered rings so far. Herein, we describe radical-mediated ring-opening and enantioselective cyanation of four- and five-membered cycloketone oxime esters to access chiral 1,5- and 1,6-dinitriles. Employment of dual photoredox/copper catalysis is essential for the asymmetric ring-opening cyanation of cyclopentanone oxime esters. Both reactions proceed under mild conditions giving chiral dinitriles in high yields and enantioselectivity with low catalyst loading and broad substrate scope. The products dinitriles can be converted to valuable optically active diamides and diamines. Mechanistic studies indicate that the benzylic radical generated via C-C single bond cleavage is involved in the catalytic cycle.
Due to high need for medical purposes, multiple harvests of mugwort (Artemisia argyi) have been extensively applied in China for the increase of mugwort yield recently. However, the investigation on ...the mineral elements in different crops, which are significantly related to mugwort growth and the clinical efficacy of this medicinal herb, has not been conducted. This study provided an analytical method and quality evaluation for mineral elements in Nanyang mugwort leaves harvested from three different crops. The contents of 35 mineral elements were determined by inductively coupled plasma mass spectrometry (ICP-MS) and inductively coupled plasma atomic emission spectrometry (ICP-AES). ANOVA, principal component analysis and factor analysis were applied to evaluate the results. Four principal components were identified and their comprehensive evaluation function was as follows: F = 0.7008Fl + 0.1236F2 + 0.0936F3 + 0.0321F4. The comprehensive scores of the mugwort leaves from different crops were ranked as follows: 3rd crop > 2nd crop ≈ 1st crop. These findings can provide a reference for the quality control and clinical use of mugwort leaves, and a guidance of differential nourishing strategies for different crops.
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