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1.
Immunity ; 44(4): 939-50, 2016 Apr 19.
Article in English | MEDLINE | ID: mdl-27067056

ABSTRACT

VRC01-class antibodies neutralize diverse HIV-1 strains by targeting the conserved CD4-binding site. Despite extensive investigations, crucial events in the early stage of VRC01 development remain elusive. We demonstrated how VRC01-class antibodies emerged in a Chinese donor by antigen-specific single B cell sorting, structural and functional studies, and longitudinal antibody and virus repertoire analyses. A monoclonal antibody DRVIA7 with modest neutralizing breadth was isolated that displayed a subset of VRC01 signatures. X-ray and EM structures revealed a VRC01-like angle of approach, but less favorable interactions between the DRVIA7 light-chain CDR1 and the N terminus with N276 and V5 glycans of gp120. Although the DRVIA7 lineage was unable to acquire broad neutralization, longitudinal analysis revealed a repertoire-encoded VRC01 light-chain CDR3 signature and VRC01-like neutralizing heavy-chain precursors that rapidly matured within 2 years. Thus, light chain accommodation of the glycan shield should be taken into account in vaccine design targeting this conserved site of vulnerability.


Subject(s)
Antibodies, Monoclonal/immunology , Antibodies, Neutralizing/immunology , Binding Sites, Antibody/immunology , HIV Antibodies/immunology , HIV Envelope Protein gp120/immunology , env Gene Products, Human Immunodeficiency Virus/immunology , Amino Acid Sequence , Broadly Neutralizing Antibodies , CD4-Positive T-Lymphocytes/immunology , HIV Infections/immunology , HIV-1/immunology , Humans , Molecular Sequence Data
2.
Anal Chem ; 96(21): 8416-8423, 2024 May 28.
Article in English | MEDLINE | ID: mdl-38755966

ABSTRACT

Nanogap-based plasmonic metal nanocrystals have been applied in surface-enhanced Raman scattering detection, while the closed and insufficient electromagnetic fields as well as the nonreproducible Raman signal of the substrate greatly restrict the actual application. Herein, a highly uniform Au/AgAu monolayer with abundant nanogaps and huge electromagnetic enhancement is prepared, which shows ultrasensitive and reproducible SERS detection. Au/AgAu with an inner nanogap is first prepared based on Au nanotriangles, and the nanogap is opened from the three tips via a subsequent etching process. The open-gap Au/AgAu displays much higher SERS efficiency than Au and Au/AgAu with an inner nanogap on detecting crystal violet due to the open-gap induced electromagnetic enhancement and improved molecular absorption. Furthermore, the open-gap Au/AgAu monolayer is prepared via interfacial self-assembly, which shows further improved SERS due to the dense and strong hotspots in the nanocavities induced by the electromagnetic coupling between adjacent open gaps. The monolayer possesses excellent signal stability, uniformity, and reproducibility. The analytic enhancement factor and relative standard deviation reach to 2.12 × 108 and 4.65% on detecting crystal violet, respectively. Moreover, the monolayer achieves efficient detection of thiram in apple juice, biphenyl-4-thiol, 4-mercaptobenzoic, melamine, and a mixed solution of four different molecules, showing great promise in practical detection.

3.
Small ; 20(14): e2308473, 2024 Apr.
Article in English | MEDLINE | ID: mdl-37972267

ABSTRACT

Decorating platinum (Pt) with a single atom offers a promising approach to tailoring their catalytic activity. In this study, for the first time, an innovative assistive active sites (AAS) strategy is proposed to construct high-loading (3.46wt.%) single Fe─N4 as AAS, which are further hybridized with small Pt nanoparticles to enhance both oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) activities. For ORR, the target catalyst (Pt/HFeSA-HCS) exhibits a higher mass activity (MA) of 0.98 A mgPt -1 and specific activity (SA) of 1.39 mA cmPt -2 at 0.90 V versus RHE. As for MOR, Pt/HFeSA-HCS shows exceptional MA (3.21 A mgPt -1) and SA (4.27 mA cmPt -2) at peak values, surpassing commercial Pt/C by 15.3 and 11.5 times, respectively. The underlying mechanism behind this AAS strategy is to find that in MOR, Fe─N4 promotes water dissociation, generating more *OH to accelerate the conversion of *CO to CO2. Meanwhile, in ORR, Fe─N4 acts as a competitor to adsorb *OH, weakening Pt─OH bonding and facilitating desorption of *OH on the Pt surface. Constructing AAS that can enhance dual functionality simultaneously can be seen as a successful "kill two birds with one stone" strategy.

4.
Small ; 20(21): e2309202, 2024 May.
Article in English | MEDLINE | ID: mdl-38100237

ABSTRACT

Histone deacetylases (HDACs) are a class of epigenetic enzymes that are closely related to tumorigenesis and suppress the expression of tumor suppressor genes. Whereas the HDACs inhibitors can release DNA into the cytoplasm and trigger innate immunity. However, the high density of chromatin limits DNA damage and release. In this study, suitable nanosized CycNHOH NPs (150 nm) and CypNHOH NPs (85 nm) efficiently accumulate at the tumor site due to the enhanced permeability and retention (EPR) effect. In addition, robust single-linear oxygen generation and good photothermal conversion efficiency under NIR laser irradiation accelerated the DNA damage process. By effectively initiating immune cell death, CypNHOH NPs activated both innate and adaptive immunity by maturing dendritic cells, infiltrating tumors with natural killer cells, and activating cytotoxic T lymphocytes, which offer a fresh perspective for the development of photo-immunotherapy.


Subject(s)
Epigenesis, Genetic , Immunotherapy , Infrared Rays , Nanoparticles , Neoplasms , Immunotherapy/methods , Epigenesis, Genetic/drug effects , Nanoparticles/chemistry , Animals , Neoplasms/therapy , Phototherapy/methods , Humans , Cell Death/drug effects , Mice , Cell Line, Tumor
5.
Plant Biotechnol J ; 22(7): 1777-1796, 2024 Jul.
Article in English | MEDLINE | ID: mdl-38348566

ABSTRACT

Heavy metal pollution poses a significant risk to human health and wreaks havoc on agricultural productivity. Phytoremediation, a plant-based, environmentally benign, and cost-effective method, is employed to remove heavy metals from contaminated soil, particularly in agricultural or heavy metal-sensitive lands. However, the phytoremediation capacity of various plant species and germplasm resources display significant genetic diversity, and the mechanisms underlying these differences remain hitherto obscure. Given its potential benefits, genetic improvement of plants is essential for enhancing their uptake of heavy metals, tolerance to harmful levels, as well as overall growth and development in contaminated soil. In this study, we uncover a molecular cascade that regulates cadmium (Cd2+) tolerance in cotton, involving GhRCD1, GhbHLH12, GhMYB44, and GhHMA1. We identified a Cd2+-sensitive cotton T-DNA insertion mutant with disrupted GhRCD1 expression. Genetic knockout of GhRCD1 by CRISPR/Cas9 technology resulted in reduced Cd2+ tolerance in cotton seedlings, while GhRCD1 overexpression enhanced Cd2+ tolerance. Through molecular interaction studies, we demonstrated that, in response to Cd2+ presence, GhRCD1 directly interacts with GhbHLH12. This interaction activates GhMYB44, which subsequently activates a heavy metal transporter, GhHMA1, by directly binding to a G-box cis-element in its promoter. These findings provide critical insights into a novel GhRCD1-GhbHLH12-GhMYB44-GhHMA1 regulatory module responsible for Cd2+ tolerance in cotton. Furthermore, our study paves the way for the development of elite Cd2+-tolerant cultivars by elucidating the molecular mechanisms governing the genetic control of Cd2+ tolerance in cotton.


Subject(s)
Cadmium , Gene Expression Regulation, Plant , Gossypium , Plant Proteins , Gossypium/genetics , Gossypium/metabolism , Cadmium/metabolism , Plant Proteins/genetics , Plant Proteins/metabolism , Gene Expression Regulation, Plant/drug effects , Biodegradation, Environmental , Plants, Genetically Modified , Transcription Factors/metabolism , Transcription Factors/genetics
6.
Chemistry ; 30(7): e202302520, 2024 Feb 01.
Article in English | MEDLINE | ID: mdl-37877456

ABSTRACT

Triplet-triplet annihilation upconversion (TTA-UC) has the potential to enhance photoredox catalysis yield. It includes a sensitizer and an annihilator. Efficient and stable annihilators are essential for photoredox catalysis, yet only a few examples are reported. Herein, we designed four novel pyrene annihilators (1, 2, 3 and 4) via introducing aryl-alkynyl groups onto pyrene to systematically modulate their singlet and triplet energies. Coupled with platinum octaethylporphyrin (PtOEP), the TTA-UC efficiency is enhanced gradually as the number of aryl-alkynyl group increases. When combining 4 with palladium tetraphenyl-tetrabenzoporphyrin (PdTPTBP), we achieved the highest red-to-green upconversion efficiency (22.4±0.3 %) (out of a 50 % maximum) so far. Then, this pair was used to activate photooxidation of aryl boronic acid under red light (630 nm), which achieved a great improved reaction yield compared to that activated by green light directly. The results not only provide a design strategy for efficient annihilators, but also show the advantage of applying TTA-UC into improving the photoredox catalysis yield.

7.
Chemistry ; 30(19): e202304081, 2024 Apr 02.
Article in English | MEDLINE | ID: mdl-38288909

ABSTRACT

Optically pure sulfoxides are valuable organosulfur compounds extensively employed in medicinal and organic synthesis. In this study, we present a biocatalytic oxidation-reduction cascade system designed for the preparation of enantiopure sulfoxides. The system involves the cooperation of a low-enantioselective chimeric oxidase SMO (styrene monooxygenase) with a high-enantioselective reductase MsrA (methionine sulfoxide reductase A), facilitating "non-selective oxidation and selective reduction" cycles for prochiral sulfide oxidation. The regeneration of requisite cofactors for MsrA and SMO was achieved via a cascade catalysis process involving three auxiliary enzymes, sustained by cost-effective D-glucose. Under the optimal reaction conditions, a series of heteroaryl alkyl, aryl alkyl and dialkyl sulfoxides in R configuration were synthesized through this "one-pot, one step" cascade reaction. The obtained compounds exhibited high yields of >90 % and demonstrated enantiomeric excess (ee) values exceeding 90 %. This study represents an unconventional and efficient biocatalytic way in utilizing the low-enantioselective oxidase for the synthesis of enantiopure sulfoxides.


Subject(s)
Methionine Sulfoxide Reductases , Sulfoxides , Biocatalysis , Oxidation-Reduction , Catalysis , Stereoisomerism
8.
BMC Cancer ; 24(1): 411, 2024 Apr 02.
Article in English | MEDLINE | ID: mdl-38566028

ABSTRACT

BACKGROUND: Deleterious BRCA1/2 (BRCA) mutation raises the risk for BRCA mutation-related malignancies, including breast, ovarian, prostate, and pancreatic cancer. Germline variation of BRCA exhibits substantial ethnical diversity. However, there is limited research on the Chinese Han population, constraining the development of strategies for BRCA mutation screening in this large ethnic group. METHODS: We profile the BRCA mutational spectrum, including single nucleotide variation, insertion/deletion, and large genomic rearrangements in 2,080 apparently healthy Chinese Han individuals and 522 patients with BRCA mutation-related cancer, to determine the BRCA genetic background of the Chinese Han population, especially of the East Han. Incident cancer events were monitored in 1,005 participants from the healthy group, comprising 11 BRCA pathogenic/likely pathogenic (PLP) variant carriers and 994 PLP-free individuals, including 3 LGR carriers. RESULTS: Healthy Chinese Han individuals demonstrated a distinct BRCA mutational spectrum compared to cancer patients, with a 0.53% (1 in 189) prevalence of pathogenic/likely pathogenic (PLP) variant, alongside a 3 in 2,080 occurrence of LGR. BRCA1 c. 5470_5477del demonstrated high prevalence (0.44%) in the North Han Chinese and penetrance for breast cancer. None of the 3 LGR carriers developed cancer during the follow-up. We calculated a relative risk of 135.55 (95% CI 25.07 to 732.88) for the development of BRCA mutation-related cancers in the BRCA PLP variant carriers (mean age 42.91 years, median follow-up 10 months) compared to PLP-free individuals (mean age 48.47 years, median follow-up 16 months). CONCLUSION: The unique BRCA mutational profile in the Chinese Han highlights the potential for standardized population-based BRCA variant screening to enhance BRCA mutation-related cancer prevention and treatment.


Subject(s)
BRCA1 Protein , Breast Neoplasms , Male , Humans , Adult , Middle Aged , BRCA1 Protein/genetics , Germ-Line Mutation , BRCA2 Protein/genetics , Genetic Predisposition to Disease , Early Detection of Cancer , China/epidemiology , Breast Neoplasms/diagnosis , Breast Neoplasms/epidemiology , Breast Neoplasms/genetics , Mutation
9.
Langmuir ; 40(16): 8327-8351, 2024 Apr 23.
Article in English | MEDLINE | ID: mdl-38606587

ABSTRACT

High emission of carbon dioxide (CO2) has caused CO2 levels to reach more than 400 ppm in air and led to a serious climate problem. In addition, in confined spaces such as submarines and aircraft, the CO2 concentration increase in the air caused by human respiration also affects human health. In order to protect the environment and human health, the search for high-performance adsorbents for carbon capture from high and low concentration gas is particularly important. Porous carbon materials, possessing the advantages of low cost and renewability, have set off a boom in the research of porous adsorbents, which have the opportunity to be utilized on a large scale for industrial carbon capture in the future. In this review, we summarize the recent research progress of porous carbons for carbon capture from flue gas and directly from air in the last five years, including activated carbon (AC), heteroatom-modified porous carbon, carbon molecular sieves (CMS), and other porous carbon materials, with a focus on the effects of temperature, water content, and gas flow rate of industrial flue gas on the performance of porous carbon adsorbents. We summarize the preparation strategies of various porous carbons and seek environmental friendly porous carbon materials preparation strategies under the premise of improving the CO2 adsorption capacity and selectivity of porous carbon adsorbents. Based on the effects of real industrial flue gas on adsorbents, we provide new ideas and evaluation methods for the development and preparation of porous carbon materials.

10.
Allergol Immunopathol (Madr) ; 52(4): 84-90, 2024.
Article in English | MEDLINE | ID: mdl-38970270

ABSTRACT

PURPOSE: To investigate the effect of metformin on gut microbiota imbalance in patients with type 2 diabetes mellitus (T2DM), and the value of probiotic supplementation. METHODS: A total of 84 newly diagnosed T2DM patients were randomly divided into probiotics group, metformin group, and control group, with 28 patients in each group. The blood glucose control, islet function, gut microbiota, and inflammatory factors were compared between three groups. RESULTS: After 3 months of treatment, fasting plasma glucose (FPG), 2-h postprandial plasma glucose (2-h PG), and glycosylated hemoglobin A1c (HbA1c) were evidently decreased in both probiotics and metformin groups (P < 0.05) and were lower than that in the control group prior to treatment. Besides, FPG, 2-h PG, and HbA1c were lower in the metformin group than that in the control group. FPG, 2-h PG, and HbA1c were further lower in the probiotic group than in the metformin group (P < 0.05). Fasting insulin (FINS) and islet ß cell (HOMA-ß) -function were dramatically increased in the same group (P < 0.05), while insulin-resistant islet ß cells (HOMA-IR) were significantly lower in the same group (P < 0.05); FINS and HOMA-ß were significantly higher, while HOMA-IR was significantly lower (P < 0.05) in both groups than in the control group prior to treatment. HOMA-IR was also lower in the probiotic group than in the metformin group after treatment (P < 0.05); the number of lactobacilli and bifidobacteria increased (P < 0.05) in both probiotic and metformin groups than in the control group prior to treatment, and the number of Enterobacteriaceae and Enterococcus was lower in the control group prior to treatment (P < 0.05). In addition, the number of lactobacilli and bifidobacteria was higher and the number of enterobacteria and enterococci was lower in the probiotic group than that in the metformin group after treatment, and the differences were statistically significant (P < 0.05). Lipopolysaccharide (LPS), interleukin 6 (IL-6), and C-reactive protein (CRP) levels were lower in both probiotic and metformin groups (P < 0.05). The serum LPS, IL-6, and CRP levels were lower in both probiotic and metformin groups, compared to the control group prior to the treatment (P < 0.05). CONCLUSION: Metformin while treating T2DM assists in improving the imbalance of gut microbiota.


Subject(s)
Blood Glucose , Diabetes Mellitus, Type 2 , Gastrointestinal Microbiome , Glycated Hemoglobin , Hypoglycemic Agents , Metformin , Probiotics , Humans , Metformin/pharmacology , Metformin/administration & dosage , Probiotics/administration & dosage , Diabetes Mellitus, Type 2/drug therapy , Diabetes Mellitus, Type 2/immunology , Diabetes Mellitus, Type 2/therapy , Diabetes Mellitus, Type 2/microbiology , Gastrointestinal Microbiome/drug effects , Gastrointestinal Microbiome/immunology , Male , Female , Middle Aged , Hypoglycemic Agents/pharmacology , Hypoglycemic Agents/administration & dosage , Hypoglycemic Agents/therapeutic use , Glycated Hemoglobin/metabolism , Blood Glucose/drug effects , Adult , Dietary Supplements , Insulin/blood , Aged
11.
Small ; 19(22): e2300200, 2023 Jun.
Article in English | MEDLINE | ID: mdl-36866464

ABSTRACT

Currently, the rarity and high cost of platinum (Pt)-based electrocatalysts seriously limit their commercial application in fuel cells cathode. Decorating Pt with atomically dispersed metal-nitrogen sites possibly offers an effective pathway to synergy tailor their catalytic activity and stability. Here active and stable oxygen reduction reaction (ORR) electrocatalysts (Pt3 Ni@Ni-N4 -C) by in situ loading Pt3 Ni nanocages with Pt skin on single-atom nickel-nitrogen (Ni-N4 ) embedded carbon supports are designed and constructed. The Pt3 Ni@Ni-N4 -C exhibits excellent mass activity (MA) of 1.92 A mgPt -1 and specific activity of 2.65 mA cmPt -2 , together with superior durability of 10 mV decay in half-wave potential and only 2.1% loss in MA after 30 000 cycles. Theoretical calculations demonstrate that Ni-N4 sites significant redistribute of electrons and make them transfer from both the adjacent carbon and Pt atoms to the Ni-N4 . The resultant electron accumulation region successfully anchored Pt3 Ni, that not only improves structural stability of the Pt3 Ni, but importantly makes the surface Pt more positive to weaken the adsorption of *OH to enhance ORR activity. This strategy lays the groundwork for the development of super effective and durable Pt-based ORR catalysts.

12.
PLoS Pathog ; 17(10): e1009968, 2021 10.
Article in English | MEDLINE | ID: mdl-34614031

ABSTRACT

Liver macrophages internalize circulating bloodborne parasites. It remains poorly understood how this process affects the fate of the macrophages and T cell responses in the liver. Here, we report that infection by Trypanosoma brucei induced depletion of macrophages in the liver, leading to the repopulation of CXCL16-secreting intrahepatic macrophages, associated with substantial accumulation of CXCR6+CD4+ T cells in the liver. Interestingly, disruption of CXCR6 signaling did not affect control of the parasitemia, but significantly enhanced the survival of infected mice, associated with reduced inflammation and liver injury. Infected CXCR6 deficient mice displayed a reduced accumulation of CD4+ T cells in the liver; adoptive transfer experiments suggested that the reduction of CD4+ T cells in the liver was attributed to a cell intrinsic property of CXCR6 deficient CD4+ T cells. Importantly, infected CXCR6 deficient mice receiving wild-type CD4+ T cells survived significantly shorter than those receiving CXCR6 deficient CD4+ T cells, demonstrating that CXCR6+CD4+ T cells promote the mortality. We conclude that infection of T. brucei leads to depletion and repopulation of liver macrophages, associated with a substantial influx of CXCR6+CD4+ T cells that mediates mortality.


Subject(s)
CD4-Positive T-Lymphocytes/immunology , Liver/immunology , Macrophages/immunology , Trypanosomiasis, African/immunology , Animals , Mice , Receptors, CXCR6/immunology , Trypanosoma brucei brucei/immunology
13.
New Phytol ; 237(4): 1100-1114, 2023 02.
Article in English | MEDLINE | ID: mdl-36352520

ABSTRACT

Cotton's fundamental requirements for long periods of growth and specific seasonal temperatures limit the global arable areas that can be utilized to cultivate cotton. This constraint can be alleviated by breeding for early-maturing varieties. By delaying the sowing dates without impacting the boll-opening time, early-maturing varieties not only mitigate the yield losses brought on by unfavorable weathers in early spring and late autumn but also help reducing the competition between cotton and other crops for arable land, thereby optimizing the cropping system. This review presents studies and breeding efforts for early-maturing cotton, which efficiently pyramid early maturity, high-quality, multiresistance traits, and suitable plant architecture by leveraging pleiotropic genes. Attempts are also made to summarize our current understanding of the molecular mechanisms underlying early maturation, which involves many pathways such as epigenetic, circadian clock, and hormone signaling pathways. Moreover, new avenues and effective measures are proposed for fine-scale breeding of early-maturing crops to ensure the healthy development of the agricultural industry.


Subject(s)
Agriculture , Plant Breeding , Phenotype , Seasons , Gossypium/genetics
14.
J Magn Reson Imaging ; 2023 Sep 25.
Article in English | MEDLINE | ID: mdl-37746892

ABSTRACT

The hip cartilage and labrum, as the main targets of femoroacetabular impingement, sports-related or traumatic damage, as well as congenital and developmental abnormalities, have attracted increasing attention with the development of magnetic resonance imaging (MRI) and hip arthroscopy. MRI is a commonly used imaging modality to noninvasively visualize the hip cartilage and labral lesions. However, conventional orthogonal MRI planes encounter unique challenges given the ball-and-socket configuration of the hip joint, its anatomically abducted and anteverted orientation, and the thin, closely apposed cartilage enveloping the femoral head and acetabulum. Advancements in hip MRI's radial plane, which is acquired through the center of the hip joint, offer a solution. This technology provides true cross-sectional images of the cartilage and labrum perpendicular to the curvature of the joint, thereby mitigating the partial-volume-averaging effects. The integration of 3.0-Tesla high field strength and three-dimensional (3D) acquisition techniques further enhances the capabilities of the radial plane. This combination yields a high signal-to-noise ratio, high spatial resolution, high contrast between intraarticular structures, while minimizing partial-volume-averaging effects. Such improvements potentially facilitate the comprehensive detection of even minor chondral and labral lesions. The capability for multiplanar reconstruction from a single 3D volumetric acquisition further strengthens the usefulness of the radial plane by aiding in precise localization of hip cartilage and labral lesions, in line with hip arthroscopy findings. These advancements have the potential to standardize MRI evaluations and radiographic reporting systems for hip cartilage and labrum, offering precise guidance for hip arthroscopy. This article presents a comprehensive review of radial plane technology applied to the hip MRI, and discusses the morphological assessment and localization of hip cartilage and labral lesions utilizing this advanced imaging technique. EVIDENCE LEVEL: 5 TECHNICAL EFFICACY: Stage 2.

15.
Langmuir ; 39(18): 6366-6374, 2023 May 09.
Article in English | MEDLINE | ID: mdl-37129291

ABSTRACT

Hydrogen gas (H2) as a fuel has the advantages of high energy density (122 kJ g-1) and zero carbon emissions. To meet the growing demand for H2 in the future, green, efficient, and convenient production technologies must be developed. The Al-H2O reaction, which produces H2 by reacting aluminum (Al) with water (H2O), is considered a rapid method for producing H2. However, Al-H2O creates a protective oxide layer on the surface of Al, preventing the production of H2. In this study, we developed a simple method for forming Al-GaInSn alloy by brushing GaInSn-Al2O3 grease onto an Al plate to form an Al/GaInSn-Al2O3/Al sandwich structure. Al2O3 in the sample supports GaInSn, prevents the leakage of GaInSn, and promotes its penetration into the Al lattice to form Al-GaInSn alloy. By forming a liquid phase within the alloy, GaInSn increases the accessibility of Al to the reaction. As a result, the Al-GaInSn alloy can rapidly react with pure H2O to produce H2 at room temperature conditions, with yields as high as ∼93.2%. It was interesting to find that dye-polluted water (methyl orange) could be synchronically purified by the Al-H2O reaction at the same time.

16.
Org Biomol Chem ; 21(16): 3417-3422, 2023 04 26.
Article in English | MEDLINE | ID: mdl-37017279

ABSTRACT

Optically pure sulfoxides are noteworthy compounds that find wide applications in various industrial fields. Here, we report a methionine sulfoxide reductase B (MsrB) homologue that exhibits high enantioselectivity and broad substrate scope for the kinetic resolution of racemic (rac) sulfoxides. This MsrB homologue, named liMsrB, was identified from Limnohabitans sp. 103DPR2 and showed good activity together with enantioselectivity towards a series of aromatic, heteroaromatic, alkyl and thioalkyl sulfoxides. Chiral sulfoxides in the S configuration were prepared in approximately 50% yield and 92-99% enantiomeric excess through kinetic resolution at an initial substrate concentration of up to 90 mM (11.2 g L-1). This study presents an efficient route for the enzymatic preparation of (S)-sulfoxides through kinetic resolution.


Subject(s)
Methionine Sulfoxide Reductases , Sulfoxides , Sulfoxides/chemistry , Kinetics , Stereoisomerism , Methionine
17.
Macromol Rapid Commun ; 44(13): e2200974, 2023 Jul.
Article in English | MEDLINE | ID: mdl-37153967

ABSTRACT

Volatile organic compounds (VOCs) may have short- and long-term adverse health effects. Especially, aromatic VOCs including benzene, toluene, ethylbenzene, and xylene (BTEX) are important indoor air pollutants. Developing highly efficient porous adsorbents with broad applicability remains a major challenge. In this study, a perchlorinated covalent-triazine framework (ClCTF-1-400) is prepared for adsorbing BTEX. ClCTF-1-400 is confirmed as a partially oxidized/chlorinated microporous covalent triazine framework through a variety of characterization. It is found that ClCTF-1-400 is reversible VOCs absorbent with very high absorption capacities, which can adsorb benzene (693 mg g-1 ), toluene (621 mg g-1 ), ethylbenzene (603 mg g-1 ), o-xylene (500 mg g-1 ), m-xylene (538 mg g-1 ), and p-xylene (592 mg g-1 ) at 25 °C and their saturated vapor pressure (≈ 1 kPa). ClCTF-1-400 is of higher adsorption capacities for all selected VOCs than activated carbon and other reported adsorbents. The adsorption mechanism is also inferred through theoretical calculation and in-site Fourier Transform Infrared (FTIR) spectroscopy. The observed excellent BTEX adsorption performance is attributed to the multiple weak interactions between the ClCTF-1-400 frameworks and aromatic molecules through multiple weak interactions (CH… π and CCl… π). The breakthrough experiment demonstrates ClCTF-1-400 has the potential for real VOCs pollutant removal in air.


Subject(s)
Volatile Organic Compounds , Benzene , Adsorption , Xylenes , Toluene
18.
Environ Res ; 239(Pt 2): 117406, 2023 Dec 15.
Article in English | MEDLINE | ID: mdl-37839529

ABSTRACT

The growing global concern about environmental threats due to environmental pollution requires the development of environmentally friendly and efficient removal/detection materials and methods. Porphyrin/phthalocyanine (Por/Pc) based porous organic polymers (POPs) as a newly emerging porous material are prepared through polymerizing building blocks with different structures. Benefiting from the high porosity, adjustable pore structure, and enzyme-like activities, the Por/Pc-POPs can be the ideal platform to study the removal and detection of pollutants. However, a systematic summary of their application in environmental treatment is still lacking to date. In this review, the development of various Por/Pc-POPs for pollutant removal and detection applications over the past decade was systematically addressed for the first time to offer valuable guidance on environmental remediation through the utilization of Por/Pc-POPs. This review is divided into two sections (pollutants removal and detection) focusing on Por/Pc-POPs for organic, inorganic, and gaseous pollutants adsorption, photodegradation, and chemosensing, respectively. The related removal and sensing mechanisms are also discussed, and the methods to improve removal and detection efficiency and selectivity are also summarized. For the future practical application of Por/Pc-POPs, this review provides the emerging research directions and their application possibility and challenges in the removal and detection of pollutants.


Subject(s)
Environmental Pollutants , Porphyrins , Environmental Pollutants/chemistry , Porosity , Polymers/chemistry
19.
Molecules ; 28(5)2023 Feb 21.
Article in English | MEDLINE | ID: mdl-36903270

ABSTRACT

Lithium-air batteries (LABs) have attracted extensive attention due to their ultra-high energy density. At present, most LABs are operated in pure oxygen (O2) since carbon dioxide (CO2) under ambient air will participate in the battery reaction and generate an irreversible by-product of lithium carbonate (Li2CO3), which will seriously affect the performance of the battery. Here, to solve this problem, we propose to prepare a CO2 capture membrane (CCM) by loading activated carbon encapsulated with lithium hydroxide (LiOH@AC) onto activated carbon fiber felt (ACFF). The effect of the LiOH@AC loading amount on ACFF has been carefully investigated, and CCM has an ultra-high CO2 adsorption performance (137 cm3 g-1) and excellent O2 transmission performance by loading 80 wt% LiOH@AC onto ACFF. The optimized CCM is further applied as a paster on the outside of the LAB. As a result, the specific capacity performance of LAB displays a sharp increase from 27,948 to 36,252 mAh g-1, and the cycle time is extended from 220 h to 310 h operating in a 4% CO2 concentration environment. The concept of carbon capture paster opens a simple and direct way for LABs operating in the atmosphere.

20.
Molecules ; 28(14)2023 Jul 24.
Article in English | MEDLINE | ID: mdl-37513478

ABSTRACT

Following the successful experimental synthesis of single-layer metallic 1T-TaS2 and semiconducting 2H-MoS2, 2H-WSe2, we perform a first-principles study to investigate the electronic and interfacial features of metal/semiconductor 1T-TaS2/2H-MoS2 and 1T-TaS2/2H-WSe2 van der Waals heterostructures (vdWHs) contact. We show that 1T-TaS2/2H-MoS2 and 1T-TaS2/2H-WSe2 form n-type Schottky contact (n-ShC type) and p-type Schottky contact (p-ShC type) with ultralow Schottky barrier height (SBH), respectively. This indicates that 1T-TaS2 can be considered as an effective metal contact with high charge injection efficiency for 2H-MoS2, 2H-WSe2 semiconductors. In addition, the electronic structure and interfacial properties of 1T-TaS2/2H-MoS2 and 1T-TaS2/2H-WSe2 van der Waals heterostructures can be transformed from n-type to p-type Schottky contact through the effect of layer spacing and the electric field. At the same time, the transition from Schottky contact to Ohmic contact can also occur by relying on the electric field and different interlayer spacing. Our results may provide a new approach for photoelectric application design based on metal/semiconductor 1T-TaS2/2H-MoS2 and 1T-TaS2/2H-WSe2 van der Waals heterostructures.

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