3D printing of poly(ethyleneimine)-functionalized Mg-Al mixed metal oxide monoliths for direct air capture of CO_(2)

Direct air capture(DAC)of CO_(2)plays an indispensable role in achieving carbon-neutral goals as one of the key negative emission technologies.Since large air flows are required to capture the ultradilute CO_(2)from the air,lab-synthesized adsorbents in powder form may cause unacceptable gas pressure drops and poor heat and mass transfer efficiencies.A structured adsorbent is essential for the implementation of gas-solid contactors for cost-and energy-efficient DAC systems.In this study,efficient adsorbent poly(ethyleneimine)(PEI)-functionalized Mg-Al-CO_(3)layered double hydroxide(LDH)-derived mixed metal oxides(MMOs)are three-dimensional(3D)printed into monoliths for the first time with more than 90%adsorbent loadings.The printing process has been optimized by initially printing the LDH powder into monoliths followed by calcination into MMO monoliths.This structure exhibits a 32.7%higher specific surface area and a 46.1%higher pore volume,as compared to the direct printing of the MMO powder into a monolith.After impregnation of PEI,the monolith demonstrates a large adsorption capacity(1.82 mmol/g)and fast kinetics(0.7 mmol/g/h)using a CO_(2)feed gas at 400 ppm at 25℃,one of the highest values among the shaped DAC adsorbents.Smearing of the amino-polymers during the post-printing process affects the diffusion of CO_(2),resulting in slower adsorption kinetics of pre-impregnation monoliths compared to post-impregnation monoliths.The optimal PEI/MeOH ratio for the post-impregnation solution prevents pores clogging that would affect both adsorption capacity and kinetics.

Rational design of vitamin C/defective carbon van der Waals heterostructure for enhanced activity,durability and storage stability toward oxygen reduction reaction

Metal-free defective carbon materials with abundant active sites have been widely studied as low-cost and efficient oxygen reduction reaction(ORR)electrocatalysts in metal-air batteries.However,the active sites in defective carbon are easily subjected to serious oxidation or hydroxylation during ORR or storage,leading to rapid degradation of activity.Herein,we design a van der Waals heterostructure comprised of vitamin C(VC)and defective carbon(DC)to not only boost the activity but also enhance the durability and storage stability of the DC-VC electrocatalyst.The formation of VC van der Waals between DC and VC is demonstrated to be an effective strategy to protect the defect active sites from oxidation and hydroxylation degradation,thus significantly enhancing the electrochemical durability and storage anti-aging performance.Moreover,the DC-VC van der Waals can reduce the reaction energy barrier to facilitate the ORR.These findings are also confirmed by operando Fourier transform infrared spectroscopy and density functional theory calculations.It is necessary to mention that the preparation of this DC-VC electrocatalyst can be scaled up,and the ORR performance of the largely produced electrocatalyst is demonstrated to be very consistent.Furthermore,the DC-VC-based aluminum-air batteries display very competitive power density with good performance maintenance.

Carbon dioxide enrichment affected flower numbers transiently and increased successful post-pollination development stably but without altering final acorn production in mature pedunculate oak (Quercus robur L.)

Acorn production in oak(Quercus spp.)shows considerable inter-annual variation,known as masting,which provides a natural defence against seed predators but a highly-variable supply of acorns for uses such as in commercial tree planting each year.Anthropogenic emissions of greenhouse gases have been very widely reported to influence plant growth and seed or fruit size and quantity via the‘fertilisation effect’that leads to enhanced photosynthesis.To examine if acorn production in mature woodland communities will be affected by further increase in CO_(2),the contents of litter traps from a Free Air Carbon Enrichment(FACE)experiment in deciduous woodland in central England were analysed for numbers of flowers and acorns of pedunculate oak(Quercus robur L.)at different stages of development and their predation levels under ambient and elevated CO_(2) concentrations.Inter-annual variation in acorn numbers was considerable and cyclical between 2015 and 2021,with the greatest numbers of mature acorns in 2015,2017 and 2020 but almost none in 2018.The numbers of flowers,enlarged cups,immature acorns,empty acorn cups,and galls in the litter traps also varied amongst years;comparatively high numbers of enlarged cups were recorded in 2018,suggesting Q.robur at this site is a fruit maturation masting species(i.e.,the extent of abortion of pollinated flowers during acorn development affects mature acorn numbers greatly).Raising the atmospheric CO_(2) concentration by 150μL L^(−1),from early 2017,increased the numbers of immature acorns,and all acorn evidence(empty cups+immature acorns+mature acorns)detected in the litter traps compared to ambient controls by 2021,but did not consistently affect the numbers of flowers,enlarged cups,empty cups,or mature acorns.The number of flowers in the elevated CO_(2) plots’litter traps was greater in 2018 than 2017,one year after CO_(2) enrichment began,whereas numbers declined in ambient plots.Enrichment with CO_(2) also increased the number of oak knopper galls(Andricus quercuscalicis Burgsdorf).We conclude that elevated CO_(2) increased the occurrence of acorns developing from flowers,but the putative benefit to mature acorn numbers may have been hidden by excessive pre-and/or post-dispersal predation.There was no evidence that elevated CO_(2) altered masting behaviour.

Boric Acid-Assisted Pyrolysis for High-Loading Single-Atom Catalysts to Boost Oxygen Reduction Reaction in Zn-Air Batteries

The emerging of single-atom catalysts(SACs)offers a great opportunity for the development of advanced energy storage and conversion devices due to their excellent activity and durability,but the actual mass production of high-loading SACs is still challenging.Herein,a facile and green boron acid(H_(3)BO_(3))-assisted pyrolysis strategy is put forward to synthesize SACs by only using chitosan,cobalt salt and H_(3)BO_(3)as precursor,and the effect of H_(3)BO_(3)is deeply investigated.The results show that molten boron oxide derived from H_(3)BO_(3)as ideal high-temperature carbonization media and blocking media play important role in the synthesis process.As a result,the acquired Co/N/B tri-doped porous carbon framework(Co-N-B-C)not only presents hierarchical porous structure,large specific surface area and abundant carbon edges but also possesses high-loading single Co atom(4.2 wt.%),thus giving rise to outstanding oxygen catalytic performance.When employed as a catalyst for air cathode in Zn-air batteries,the resultant Co-N-B-C catalyst shows remarkable power density and long-term stability.Clearly,our work gains deep insight into the role of H_(3)BO_(3)and provides a new avenue to synthesis of high-performance SACs.

Vonoprazan-amoxicillin dual regimen with Saccharomyces boulardii as a rescue therapy for Helicobacter pylori:Current perspectives and implications

Yu et al’s study in the World Journal of Gastroenterology(2023)introduced a novel regimen of Vonoprazan-amoxicillin dual therapy combined with Saccharomyces boulardii(S.boulardii)for the rescue therapy against Helicobacter pylori(H.pylori),a pathogen responsible for peptic ulcers and gastric cancer.Vonoprazan is a potassium-competitive acid blocker renowned for its rapid and long-lasting acid suppression,which is minimally affected by mealtime.Compared to proton pump inhibitors,which bind irreversibly to cysteine residues in the H+/K+-ATPase pump,Vonoprazan competes with the K+ions,prevents the ions from binding to the pump and blocks acid secretion.Concerns with increasing antibiotic resistance,effects on the gut microbiota,patient compliance,and side effects have led to the advent of a dual regimen for H.pylori.Previous studies suggested that S.boulardii plays a role in stabilizing the gut barrier which improves H.pylori eradication rate.With an acceptable safety profile,the dual-adjunct regimen was effective regardless of prior treatment failure and antibiotic resistance profile,thereby strengthening the applicability in clinical settings.Nonetheless,S.boulardii comes in various formulations and dosages,warranting further exploration into the optimal dosage for supplementation in rescue therapy.Additionally,larger,randomized,double-blinded controlled trials are warranted to confirm these promising results.

Synthesis of phosphonated graphene oxide by electrochemical exfoliation to enhance the performance and durability of high-temperature proton exchange membrane fuel cells

The doping of functionalized graphene oxide(GO)in the membranes becomes a promising method for improving the performance of high-temperature proton exchange membrane fuel cells(HT-PEMFC).Phosphonated graphene oxide(PGO)with a P/O ratio of 8.5%was quickly synthesised by one-step electrochemical exfoliation based on a three-dimensiaonal(3D)printed reactor and natural graphite flakes.Compared with the GO prepared by the two-step electrochemical exfoliation method,the PGO synthesized by the one-step electrochemical exfoliation can better improve the performance of the membrane-electrode-assembly(MEA)based on the polybenzimidazole(PBI)membrane in the HTPEMFC.The doping of 1.5 wt%GO synthesised by electrochemical exfoliation with the 2-step method or reactor method in PBI increased the peak power density by 17.4%or 35.4%compared to MEA based on pure PBI membrane at 150℃,respectively.In addition,the doping of PGO in PBI improves its durability under accelerated stress test(AST).

Ultra-thin Oxide Films on SiO_2: An STM Study of Their Thermal Stability in the Presence of Au Deposit

The annealing of Au particles deposited onto the ultrathin layers of SiO 2 on Si(111) has been studied in real time with a high temperature scanning tunnelling microscopy. Annealing did not create significant changes to the morphology of the surface until the surface was heated up to more than 920 K when the gold particles started to display a preference for the step edge. Further heating caused the decomposition of the oxide layer with the formation of voids on the surface in the surface step edge area. Comparison between the gold assisted oxide decomposition and pure oxide decomposition indicates that the two decomposition routes proceed with different mechanisms.

Dehydration of sugars to 5-hydroxymethylfurfural and non-stoichiometric formic and levulinic acids over mesoporous Ta and Ta-W oxide solid acid catalysts

A series of mesoporous Ta and Ta-W oxides have been prepared and employed as solid acid catalysts for the dehydration of fructose and glucose to 5-hydroxymethylfurfural(HMF).Solid state 31 P MAS NMR spectroscopic results using trimethylphosphine(TMP)as a probe molecule show that the acid strength and the ratio of Br?nsted to Lewis acid sites increase gradually with the addition of tungsten in tantalum oxide.It is found that high sugar conversion and HMF selectivity are achieved over catalyst with relatively high ratios of Br?nsted to Lewis acid sites.Unexpected stoichiometric excess of formic acid relative to levulinic acid can be observed mainly because of direct decomposition of fructose over Lewis acid sites.The addition of 2-butanol leads to the increase of sugars conversion and the HMF selectivity,especially for the catalyst with high ratio of Br?nsted to Lewis acid sites.Among them,Ta7W3 oxide catalyst shows 54%HMF selectivity and good reusability with the addition of 2-butanol by extracting HMF from aqueous phase and removing humins deposed on the surface of the catalyst.

Investigation on High Efficient Catalysts for the Oxidative Dehydrogenation of Ethane

Since the pioneer work of Thorsteinson fot me ox（?） ethane, a series of V-Mo based catalysts mainly for the oxidative dehydrogenation of ethane have been patented. On the surfaces of these catalysts, a C;H;selectivity of 70％ was achieved, but the space velocity was only about 340 h;. Lunsford, et al. reported a C;H;conversion of 75％ and a C;H;selectivity of 76％ over the

Measurement of total phenolic content and antioxidant activity of aerial parts of medicinal plant Coronopus didymus

Objective: To evaluate the total phenolic content and compare the antioxidant activity of various solvent extracts and fractions from the aerial parts of Coronopus didymus through various assays. Methods: Total phenolic content was determined using the Folin-Ciocalteu assay and the in vitro antioxidant activity of a number of different extracts was investigated in a dose-dependent manner with three different methods: the 2,2-diphenyl-1-picrylhydrazyl(DPPH), 2,2'-azinobis(3-ethylbenzothiazoline-6-sulfonic acid) diammonium salt(ABTS) and ferric reducing antioxidant power(FRAP) assays. A flavone was isolated from the most active ethanolic extract with high antioxidant activity using size exclusion chromatography. IC_(50) values were calculated for the DPPH and ABTS methods. The FRAP activity was assessed in terms of μM Fe(II) equivalent. Results: The phenolic content was found to be highest in the ethanol extract(CDA Et; 47.8 mM GAE) and the lowest in the dichloromethane extract(CDA DCM; 3.13 mM GAE). The ethanol extract showed high radical scavenging activity towards DPPH and ABTS radicals with IC_(50) values of(7.80 × 10~2) and(4.32 × 10~2) μg/m L, respectively. The most active ethanol extract had a FRAP value of 1 921.7 μM Fe(Ⅱ) equivalent. The isolated flavone F10C(5,7,4'-trihydroxy-3'-methoxy flavone) was far more effective for scavenging free radicals in the DPPH and ABTS assays with IC_(50) of 43.8 and 0.08 μg/m L, than the standard trolox, with IC_(50) values of 97.5 and 21.1 μg/m L, respectively. In addition, the flavone F10C and the standard ascorbic acid had FRAP values of 1 621.7 and 16 038.0 μM Fe(Ⅱ) equivalents, respectively. Conclusions: The total phenolic content of extracts in decreasing order is ethanol extract(CDA Et)> acetone extract(CDA ACE)> phenolic extract(CDA MW)> n-hexane extract(CDA nHX)> chloroform extract(CDA CHL)> dichloromethane extract(CDA DCM). The ordering of extracts in terms of antioxidant activity from highest to lowest is CDA Et> CDA MW> CDA DCM> CDA CHL> CDA ACE> CDA nHX in DPPH, ABTS and FRAP assays. A significant relationship is found between antioxidant potential and total phenolic content, suggesting that phenolic compounds are the major contributors to the antioxidant activity of Coronopus didymus.

Analysis of the Hox epigenetic code

Archetypes of histone modifications associated with diverse chromosomal states that regulate access to DNA are leading the hypothesis of the histone code(or epigenetic code). However, it is still not evident how these post-translational modifications of histone tails lead to changes in chromatin structure. Histone modifications are able to activate and/or inactivate several genes and can be transmitted to next generation cells due to an epigenetic memory. The challenging issue is to identify or "decrypt" the code used to transmit these modifications to descent cells. Here, an attempt is made to describe how histone modifications operate as part of histone code that stipulates patterns of gene expression. This papers emphasizes particularly on the correlation between histone modifications and patterns of Hox gene expression in Caenorhabditis elegans. This work serves as an example to illustrate the power of the epigenetic machinery and its use in drug design and discovery.

Syntheses and Bioactivities of 4-Ar-2-oxo-glutaric Acids

Fourteen novel compounds were synthesized and characterized by using NMR and ESI-MS methods. The bioactivities of the four novel 4-Ar-2-oxo-glutaric acids were studied by using the LC-MS method. The experimental results show that 3-nitrobenzyl-2-oxo-glutaric acid is a mild inhibitor for the hydroxylation reaction catalyzed by PHD2. The decarboxylated peak for 3-fluorobenzyl-2-oxo-glutaric acid was observed by using the negative LC-MS method, indicating that it can be used as a mild cosubstrate to replace 2-OG, but this is possible only in the presence of the prime peptide CODD 19 mer.

Ti-modified Mesoporous Molecular Sieves Containing both Selective Oxidation and Photocatalysis Centers

Mesoporous molecular sieves possessing high mesopore volumes and large specific surface areas were prepared and characterized by means of XRD, low temperature N_2 adsorption-desorption measurements, FT IR, Raman, UV-visible diffuse reflectance and XPS spectroscopy. The materials contain both framework and extra-framework Ti centers which exhibit selective oxidation catalytic activity and photocatalytic activity respectively. The catalysis of selective oxidation was studied with the hydroxylation of benzene with hydrogen peroxide and photochemical activity was studied by the yields of ·OH and H_2O_2, respectively.

Synthesis and Bioassay of 4-Substituted 2-Oxoglutaric Acids

Three 2-oxoglutaric acid analogues were synthesized. Their interaction with factor- inhibiting hypoxia-inducible factor （FIH） was studied using LC-MS method. The results show that hydrophobic substitutes of 2-oxoglutaric acids have great influence on their inhibitor activity.

Selective Oxidation of PM over Li Doped Potassium Titanate Catalysts

K2Ti2O5 and LixK2-xTi2O5 samples with varying K contents （x=0.125, 0.15, 0.3）, targeted on removal of two main environmental pollutants： PM and NOx, were synthesized by the solid state method using TiO2, KNO3 and LiOH-H2O as starting materials and were characterized by X-ray diffractometry, scanning electron microscopy, and BET. The catalytic activity of titanate catalysts on PM oxidation was evaluated using the temperature programmed oxidation （TPO） method. The test results showed that the perovskite structure of K2Ti205 was still retained after doping a small amount of Li, and the catalytic performance of LixK2-xTi2O5 had been improved significantly compared with that of K2Ti2O5. Li0.15K1.85Ti205 catalyst had the highest catalytic activity with an ignition temperature of 210℃ and a peak temperature of 290℃. The catalytic activity of both K2Ti2O5 and LixK2-xTi2O5 under intimate contact was higher than that under loose contact. When the exhaust gas flow rate was around 100 mL/min, the catalyst samples showed a highest activity. The Li doped K2Ti2O5 could be an excellent candidate for PM oxidation due to its high oxidation activity, water stability, resistance to sulfur poisoning and economical advantages.

Tungsten Promoted Ni/Al_2O_3 Catalysts for Carbon Dioxide Reforming of Methane to Synthesis Gas

A series of tungsten promoted alumina supported nickel catalysts has been prepared for the carbon dioxide reforming of methane to synthesis gas. The catalysts have been characterized by means of XRD, TEM, and Laser Raman spectroscopy. It is shown that the addition of tungsten to the nickel catalyst can stabilize the catalyst and increase the resistance to carbon deposition. Adding a suitable amount of tungsten can also increase the catalyst activity to be close to that of supported noble metal catalysts. The carburisation of the tungsten modified nickel catalyst decreases the catalyst activity at lower reaction temperatures(<1123K), but has no effect on the catalyst performance at higher reaction temperatures. The alumina supported nickel catalyst modified by 0.67%(mass fraction) WO_3 has the equivalent equilibrium constant of the dry reforming reaction to that of alumina supported 5%(mass fraction) Ru at 873 K, and also has a lower activation energy for dry reforming than the latter.

Probe-assisted NMR:Recent progress on the surface study of crystalline metal oxides with various terminated facets

The development of metal oxides with specific facet exposure for better catalytic performance in targeted applications has been well-documented.However,the understanding of surface structure-activity correlation is severely hindered by the current poor resolution of conventional surface characterization tools.In this mini-review,some of the latest research developments on the characterization of the surface structure and properties of faceted ZnO and TiO_(2)by probe-assisted nuclear magnetic resonance spectroscopy(NMR)are discussed.

Interfacial oxidized Pd species dominate catalytic hydrogenation of polar unsaturated bonds

The determination of catalytically active sites is crucial for the design of efficient and stable catalysts toward desired reactions.However,the complexity of supported noble metal catalysts has led to controversy over the locations of catalytically active sites(e.g.,metal,support,and metal/support interface).Here we develop a structurally controllable catalyst system(Pd/SBA-15)to reveal the catalytic active sites for the selective hydrogenation of ketones to alcohol using acetophenone hydrogenation as model reaction.Systematic investigations demonstrated that unsupported Pd nanocrystals have no catalytic activity for acetophenone hydrogenation.However,oxidized Pd species were catalytically highly active for acetophenone hydrogenation.The catalytic activity decreased with the decreased oxidation state of Pd.This work provides insights into the hydrogenation mechanism of ketones but also other unsaturated compounds containing polar bonds,e.g.,nitrobenzene,N-benzylidene-benzylamine,and carbon dioxide.

Constraining the links between the Himalayan belt and the Central Myanmar Basins during the Cenozoic:An integrated multi-proxy detrital geochronology and trace-element geochemistry study

Geological and tectonic analysis of the Eastern Himalayan basins has given rise to a decade-long debate on the geodynamic evolution of the Burmese terrane and on the extent of reorganization of the main SE Asia drainage systems.However,the influence of the Himalayan belt on the Central Myanmar Basin(CMB)system remains poorly documented,although it is key to providing more accurate models for the evolution of the Himalayan-Burmese orogen.In this contribution,we present geochronological,isotopic and geochemical analysis from 2500 zircon,1700 titanite,700 rutile and 850 apatite detrital grains from fifteen Cenozoic siliciclastic samples and one Cretaceous igneous rock.The samples were collected within the fore-and back-arc basins of the Central Myanmar Basin domain(CMB)to constrain the provenance,maximum depositional ages,and depositional environments of the west Burma terrane.Nine key lithological units,the Sadwingyi,Ketpanda,Wabo Chaung,Gwegon,Minwun,Padaung,Okmintaung and Irrawaddy formations have detrital age spectra spanning from the Miocene to Paleoarchean.The entire data set has common age peaks at ca.20,40,60,90,100 Ma,with about 80%of the U–Pb ages younger than ca.140 Ma and only ca.1%of the grains predating ca.3.0 Ga.Our results shed light on the current ambiguities on the transport pathways of Himalayan detritus in the CMB.They show that the fore-arc basin was open to the trench and fed by the unroofing of both the Wuntho Popa volcanic arc to the east and possibly from the Burmese basement and/or from Himalayan-derived Bengal Fan detritus to the west during the Eocene,from at least ca.44 Ma to before ca.39 Ma.We show that the west Burma Terrane was partitioned into pull-apart basins such as the Minwun Basin,which during the Oligocene recorded the first evidence of a new source contribution into the CMB at ca.27 Ma.This new source is characterized by detritus highly compatible with the SE Asia basement rocks,which we suggest corresponds to the initiation of the palaeo–Irrawaddy River.This geodynamic evolution does not require any Yarlung Tsangpo-Irrawaddy-Brahmaputra paleodrainage reorganization,since from the Oligocene to the Early Miocene,the Irrawaddy River fed an internally drained basin,and from the Late Miocene onwards,the Yarlung drained into the Brahmaputra in the Bengal Basin.

Development of a Novel, Oxidatively Activated, Safety-Catch Linker for Solid-Phase Asymmetric Organic Synthesis (SPOS)

Solid-phase asymmetric organic synthesis has become a very important synthetic strategy within the organic chemistry community.[1] Critical to success in SPOS is a linking strategy which allows both the substrate to be loaded and the product released efficiently from the polymeric support. A safety catch linker[2] (SCL) is in principle a linking molecule orthogonal to the reaction conditions of the library synthesis, which can be easily activated by a simple chemical transformation to allow efficient cleavage of the products from the polymer under mild conditions. In order to introduce the SuperQuat chiral auxiliaries[3] for SOPS, we report herein design and synthesis of a novel safety catch linker for asymmetric conjugate addition reactions.……