Templated synthesis of transition metal phosphide electrocatalysts for oxygen and hydrogen evolution reactions

Transition metal phosphides(TMPs)have been regarded as alternative hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts owing to their comparable activity to those of noble metal-based catalysts.TMPs have been produced in various morphologies,including hollow and porous nanostructures,which are features deemed desirable for electrocatalytic materials.Templated synthesis routes are often responsible for such morphologies.This paper reviews the latest advances and existing challenges in the synthesis of TMP-based OER and HER catalysts through templated methods.A comprehensive review of the structure-property-performance of TMP-based HER and OER catalysts prepared using different templates is presented.The discussion proceeds according to application,first by HER and further divided among the types of templates used-from hard templates,sacrificial templates,and soft templates to the emerging dynamic hydrogen bubble template.OER catalysts are then reviewed and grouped according to their morphology.Finally,prospective research directions for the synthesis of hollow and porous TMP-based catalysts,such as improvements on both activity and stability of TMPs,design of environmentally benign templates and processes,and analysis of the reaction mechanism through advanced material characterization techniques and theoretical calculations,are suggested.

Navigating the pathways:TAR-DNA-binding-protein-43 aggregation,axonal transport,and local synthesis in amyotrophic lateral sclerosis pathology

Neurons are highly polarized cells with axons reaching over a meter long in adult humans.To survive and maintain their proper function,neurons depend on specific mechanisms that regulate spatiotemporal signaling and metabolic events,which need to be carried out at the right place,time,and intensity.Such mechanisms include axonal transport,local synthesis,and liquid-liquid phase separations.Alterations and malfunctions in these processes are correlated to neurodegenerative diseases such as amyotrophic lateral sclerosis(ALS).

Synthesis and Modulation of Low-Dimensional Transition Metal Chalcogenide Materials via Atomic Substitution

In recent years,low-dimensional transition metal chalcogenide(TMC)materials have garnered growing research attention due to their superior electronic,optical,and catalytic properties compared to their bulk counterparts.The controllable synthesis and manipulation of these materials are crucial for tailoring their properties and unlocking their full potential in various applications.In this context,the atomic substitution method has emerged as a favorable approach.It involves the replacement of specific atoms within TMC structures with other elements and possesses the capability to regulate the compositions finely,crystal structures,and inherent properties of the resulting materials.In this review,we present a comprehensive overview on various strategies of atomic substitution employed in the synthesis of zero-dimensional,one-dimensional and two-dimensional TMC materials.The effects of substituting elements,substitution ratios,and substitution positions on the structures and morphologies of resulting material are discussed.The enhanced electrocatalytic performance and photovoltaic properties of the obtained materials are also provided,emphasizing the role of atomic substitution in achieving these advancements.Finally,challenges and future prospects in the field of atomic substitution for fabricating low-dimensional TMC materials are summarized.

Metagenomic analysis revealing the metabolic role of microbial communities in the free amino acid biosynthesis of Monascus rice vinegar during fermentation

Free amino acid(FAA)is the important component of vinegar that infl uences quality perception and consumer acceptance.FAA is one of the major metabolites produced by microorganisms;however,the microbial metabolic network on FAA biosynthesis remains unclear.Through metagenomic analysis,this work aimed to elucidate the roles of microbes in FAA biosynthesis during Monascus rice vinegar fermentation.Taxonomic profiles from functional analyses showed 14 dominant genera with high contributions to the metabolism pathways.The metabolic network for FAA biosynthesis was then constructed,and the microbial distribution in different metabolic pathways was illuminated.The results revealed that 5 functional genera were closely involved in FAA biosynthesis.This study illuminated the metabolic roles of microorganisms in FAA biosynthesis and provided crucial insights into the functional attributes of microbiota in vinegar fermentation.

Recent advances in the synthesis, characterization, and catalytic consequence of metal species confined within zeolite for hydrogen-related reactions

Zeolites-encapsulated metal and metal oxide species are important heterogeneous catalysts.They give performances that steadily outperform traditional supported catalysts in many important reactions and have become a research hotspot.Remarkable achievements have been made with respect to the synthesis,characterization,and performances of metal species(typically metal and metal oxide clusters)confined in zeolites.The development in the strategies for the encapsulation of metal species including posttreatment and in situ synthesis method are introduced and compared.For the characterization of zeoliteencapsulated metal catalysts,the structural and surface properties of metal species are studied by several useful techniques,such as electron microscopy,X-ray absorption(XAS),Fourier transform infrared spectroscopy of CO(FTIR-CO),and chemisorption,which confirm the successful confinement of metal species in zeolites and their unique physiochemical properties.In addition,the encapsulation fraction can be determined by a probe molecular titration reaction.For the catalytic performance of zeoliteencapsulated metal catalysts,the activity,selectivity,and stability are emphasized.Finally,applications of zeolite-encapsulated metal catalysts in hydrogen-related reactions are summarized.

Transcriptomic and metabolomic analysis provides insights into lignin biosynthesis and accumulation and differences in lodging resistance in hybrid wheat

The use of hybrid wheat is one way to improve the yield in the future.However,greater plant heights increase lodging risk to some extent.In this study,two hybrid combinations with differences in lodging resistance were used to analyze the stem-related traits during the filling stage,and to investigate the mechanism of the difference in lodging resistance by analyzing lignin synthesis of the basal second internode(BSI).The stem-related traits such as the breaking strength,stem pole substantial degree(SPSD),and rind penetration strength(RPS),as well as the lignin content of the lodging-resistant combination(LRC),were significantly higher than those of the lodgingsensitive combination(LSC).The phenylpropanoid biosynthesis pathway was significantly and simultaneously enriched according to the transcriptomics and metabolomics analysis at the later filling stage.A total of 35 critical regulatory genes involved in the phenylpropanoid pathway were identified.Moreover,42%of the identified genes were significantly and differentially expressed at the later grain-filling stage between the two combinations,among which more than 80%were strongly up-regulated at that stage in the LRC compared with LSC.On the contrary,the LRC displayed lower contents of lignin intermediate metabolites than the LSC.These results suggested that the key to the lodging resistance formation of LRC is largely the higher lignin synthesis at the later grain-filling stage.Finally,breeding strategies for synergistically improving plant height and lodging resistance of hybrid wheat were put forward by comparing the LRC with the conventional wheat applied in large areas.

A perspective review on the biosynthesis of plant-based secondary metabolites and their application as potent drugs

Many phytochemicals and their derived metabolites produced by plants are extensively employed in commercial goods,pharmaceutical products as well as in the environmental and medicalfields.However,these secondary metabolites obtained from plants are in low amounts,and it is difficult to synthesize them at the industrial level.Despite these challenges,they may be utilized for a variety of medicinal products that are either available in the market or are being researched and tested.Secondary metabolites are complex compounds that exhibit chirality.Further,under controlled conditions with elicitors,desired secondary metabolites may be produced from plant cell cultures.This review emphasizes the various aspects of secondary metabolites including their types,synthesis,and applications as medicinal products.The article aims to promote the use of plant secondary metabolites in the management and treatment of various diseases.

Porous TiFe_(2) intermetallic compound fabricated via elemental powder reactive synthesis

Porous intermetallics show potential in the field of filtration and separation as well as in the field of catalysis.Herein,porous Ti Fe2intermetallics were fabricated by the reactive synthesis of elemental powders.The phase transformation and pore formation of porous TiFe2intermetallics were investigated,and its corrosion behavior and hydrogen evolution reaction(HER)performance in alkali solution were studied.Porous TiFe2intermetallics with porosity in the range of 34.4%-56.4%were synthesized by the diffusion reaction of Ti and Fe elements,and the pore formation of porous TiFe2intermetallic compound is the result of a combination of the bridging effect and the Kirkendall effect.The porous TiFe2samples exhibit better corrosion resistance compared with porous 316L stainless steel,which is related to the formation of uniform nanosheets on the surface that hinder further corrosion,and porous TiFe2electrode shows the overpotential of 220.6 and 295.6 mV at 10 and 100 mA·cm-2,suggesting a good catalytic performance.The synthesized porous Fe-based intermetallic has a controllable pore structure as well as excellent corrosion resistance,showing its potential in the field of filtration and separation.

Electrochemical synthesis of trimetallic nickel-iron-copper nanoparticles via potential-cycling for high current density anion exchange membrane water-splitting applications

Hydrogen is known for its elevated energy density and environmental compatibility and is a promising alternative to fossil fuels.Alkaline water electrolysis utilizing renewable energy sources has emerged as a means to obtain high-purity hydrogen.Nevertheless,electrocatalysts used in the process are fabricated using conventional wet chemical synthesis methods,such as sol-gel,hydrothermal,or surfactantassisted approaches,which often necessitate intricate pretreatment procedures and are vulnerable to post-treatment contamination.Therefore,this study introduces a streamlined and environmentally conscious one-step potential-cycling approach to generate a highly efficient trimetallic nickel-iron-copper electrocatalyst in situ on nickel foam.The synthesized material exhibited remarkable performance,requiring a mere 476 mV to drive electrochemical water splitting at 100 mA cm^(-2)current density in alkaline solution.Furthermore,this material was integrated into an anion exchange membrane watersplitting device and achieved an exceptionally high current density of 1 A cm^(-2)at a low cell voltage of2.13 V,outperforming the noble-metal benchmark(2.51 V).Additionally,ex situ characterizations were employed to detect transformations in the active sites during the catalytic process,revealing the structural transformations and providing inspiration for further design of electrocatalysts.

Synthesis of high-capacity LiNi_(0.8)Co_(0.1)Mn_(0.1)O_2 cathode by transition metal acetates

LiNi0.8Co0.1Mn0.1O2 cathode was synthesized using transition metal acetates under different synthesis conditions. Simultaneous thermogravimetric–differential scanning calorimetry–derivative thermogravimetric analysis was applied to investigating the mixture of transition metal acetates. X-ray powder diffraction and charge–discharge test were adopted to characterize the as-prepared LiNi0.8Co0.1Mn0.1O2. The mixture of transition metal acetates undergoes dehydration and decomposition during heating. All the examined LiNi0.8Co0.1Mn0.1O2 samples have a layered structure with R3 m space group. LiNi0.8Co0.1Mn0.1O2 samples prepared with different lithium sources under different synthesis conditions exhibit very different charge–discharge performances. The sample synthesized via the procedure of sintering at 800 °C after heating lithium carbonate and transition metal acetates at 550 °C achieves a highest capacity of 200.8 m A·h/g and an average capacity of 188.1 mA ·h/g in the first 20 cycles at 0.2C.

Novel synthesis metal 3-alkylthiophene copolymer

Copolymer, regiorandom and regioregular poly （ 3-octylthiophene ）-co-poly （ 3-（ 2-ethyl-1- hexylthiophene））（P3OTIOT） was synthesized by a FeCl3-oxidation and GRIM （grignard method） approach. The structure and optical properties were verified by the Fourier transform infrared, ultraviolet visible spectroscopy, NMR （nuclear magnetic resonance ）, gel permeation chromatography （GPC） and photoluminescence （PL）. The results indicate that the band-gap energy of the regioregular HT P3OTEHT was lower than that of the regiorandom copolymer and both of them depict low band-gap energy, high photoluminescence quantum yield, excellent solubility and processability, and might be promising polymer materials for applications in polymer light-emitting diodes, light-emitting electrochemical cells and polymer solar cells, etc.

运动疗法对前交叉韧带重建后康复疗效影响的网状Meta分析

目的:运动干预被认为是前交叉韧带重建后康复的基础。然而,关于何种运动疗法在改善前交叉韧带重建后患者膝关节肌肉力量和功能方面更有效,目前仍未得出明确结论。为此,文章采用网状Meta分析方法,比较运动疗法治疗前交叉韧带重建后的疗效,为选择最佳运动疗法提供循证医学依据。方法:计算机检索PubMed,Web of Science,Embase,The Cochrane Library及EBSCO数据库运动疗法治疗前交叉韧带重建后的随机对照试验,检索时限均从建库至2023-11-20。结局指标包括股四头肌肌力、腘绳肌肌力、膝关节功能评分3个连续性变量。运用EndNote X9.1软件筛选文献。采用Cochrane风险偏倚评估工具对纳入的文献进行质量评价,根据GRADE评分对文章结果的证据强度进行评级,采用Stata 16.0进行网状Meta分析。结果:①共纳入36项随机对照试验,包括1179例前交叉韧带重建后患者,纳入文献整体质量中等;涉及9种运动疗法:等速训练、交叉训练、离心训练、水中康复、血流限制训练、运动控制训练、增强式训练、全身振动训练和综合训练;对照措施为常规康复训练。②网状Meta分析结果显示:与常规康复训练相比,离心训练(SMD=2.08,95%CI:0.56-3.60,P=0.007)对前交叉韧带重建后患者股四头肌肌力的改善效果最佳,其次是综合训练(SMD=1.69,95%CI:0.11-3.27,P=0.249)和全身振动训练(SMD=0.81,95%CI:0.11-1.51,P=0.042);在提升患者腘绳肌肌力方面,综合训练(SMD=2.08,95%CI:0.30-3.86,P=0.022)效果最佳,其次是增强式训练(SMD=1.51,95%CI:0.18-2.84,P=0.026)和等速训练(SMD=1.37,95%CI:0.06-2.67,P=0.039);综合训练(SMD=4.60,95%CI:2.40-6.80,P<0.001)改善膝关节功能评分最有效,其次是离心训练(SMD=1.75,95%CI:0.24-3.25,P=0.023)和水中康复(SMD=1.65,95%CI:0.07-3.24,P=0.041)。结论:低到中等强度的临床证据证实,在改善前交叉韧带重建后患者膝关节肌肉力量和功能方面,综合训练可能是最有效的运动疗法,其次是离心训练、增强式训练、等速训练、全身振动训练、水中康复。未来仍需更多高质量的临床随机对照试验来验证结论的可靠性。

颈前路减压融合ROI-C^(TM)自锁系统治疗退行性颈椎病的Meta分析

目的:颈前路减压融合术是治疗退行性颈椎病的经典手术方式,钉板的使用增加了融合率及稳定性的同时,间接导致了邻近椎体退变和术后吞咽困难的发生。文章通过Meta分析方法比较ROI-C^(TM)自锁系统和传统融合器联合钉板内固定治疗退行性颈椎病患者的临床结果和并发症情况,为颈前路减压融合术中内固定方式的选择提供循证学支持。方法:检索中国知网、万方、维普、PubMed、Cochrane Library、Web of Science和Embase数据库,检索关于颈前路减压融合术中应用ROI-C^(TM)自锁系统与融合器联合钉板内固定治疗退行性颈椎病的中英文文献。检索时间范围为各数据库建库至2023年7月。由2名研究者严格按照纳入与排除标准选择文献,采用Cochrane偏倚风险工具对随机对照试验进行质量评价,NOS量表对队列研究进行质量评价。采用RevMan 5.4软件进行Meta分析。结局指标包括手术时间、术中出血量、日本骨科协会(Japanese Orthopaedic Association Scores,JOA)评分、颈椎功能障碍指数、C_(2)-C_(7)Cobb角、融合率、邻近椎体退变发生率、融合器沉降率和吞咽困难发生率。结果:共纳入13项研究,其中回顾性队列研究11项,随机对照试验2项,共1136例患者,ROI-C组569例,融合器联合钉板组567例。Meta分析结果显示:ROI-C组与融合器联合钉板组在手术时间(MD=-15.52,95%CI:-18.62至-12.42,P<0.00001),术中出血量(MD=-24.53,95%CI:-32.46至-16.61,P<0.00001),术后邻近节段退变率(RR=0.40,95%CI:0.27-0.60,P<0.00001)和术后总吞咽困难发生率(RR=0.18,95%CI:0.13-0.26,P<0.00001)均具有显著性差异。两者在术后JOA评分、颈椎功能障碍指数、C_(2)-C_(7)Cobb角、融合率和融合器沉降率方面无显著性差异(P≥0.05)。结论:在颈椎前路减压融合术中应用ROI-C^(TM)自锁系统与传统融合器联合钉板内固定治疗退行性颈椎病均可达到满意的临床效果,ROI-C^(TM)自锁系统操作更加简单,相比融合器联合钉板内固定能明显减少手术时间及术中出血量,在减少术后吞咽困难及邻近节段退变发生率等方面具有明显优势,对于跳跃型颈椎病及邻椎病翻修患者,更加推荐使用ROI-C^(TM)自锁系统。但鉴于其可能存在较高的沉降率,对于多节段且合并融合器沉降高危因素如骨质疏松、椎体终板破损的退行性颈椎病患者,仍建议使用融合器联合钉板内固定。

The structure-directing role of heterologous seeds in the synthesis of zeolite

Zeolites have been widely used as catalysts,ion-exchangers,and adsorbents in chemical industries,detergent industry,steel industry,glass industry,ceramic industry,medical and healthfield,and environmentalfield,and recently applied in energy storage.Seed-assisted synthesis is a very effective approach in promoting the crystallization of zeolites.In some cases,the target zeolite cannot be formed in the absence of seed zeolite.In homologous seed-assisted synthesis,the structure of the seed zeolite is the same to that of the target zeolite,while the structure of the seed zeolite is different to that of the target zeolite in the heterologous seed-assisted synthesis.In this review,we briefly summarized the heterologous seed-assisted syntheses of zeolites and analyzed the structure-directing effect of heterologous seeds and surveyed the“common composite building units(CBUs)hypothesis”and the“common secondary building units(SBUs)hypothesis”.However,both hypotheses cannot explain all observations on the heterologous seed-assisted syntheses.Finally,we proposed that the formation of the target zeolite does need nuclei with the structure of target zeolite and the formation of the nuclei of the target zeolite can be promoted by either the undissolved seed crystals with the same CBUs or SBUs to the target zeolite or by the facilitated appropriate distribution of the specific building units due to the presence of the heterologous seed that does not have any common CBUs and SBUs with the target zeolite.

Facile synthesis of hierarchical NaX zeolite from natural kaolinite for efficient Knoevenagel condensation

Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficiency.Herein,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical 2-cyano-3-phenylacrylate.The synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or seed.Systematic characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX zeolite.Detailed mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized kaolinite.This synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.

Optimal synthesis of heat-integrated distillation configurations using the two-column superstructure

In the realm of the synthesis of heat-integrated distillation configurations,the conventional approach for exploring more heat integration possibilities typically entails the splitting of a single column into a twocolumn configuration.However,this approach frequently necessitates tedious enumeration procedures,resulting in a considerable computational burden.To surmount this formidable challenge,the present study introduces an innovative remedy:The proposition of a superstructure that encompasses both single-column and multiple two-column configurations.Additionally,a simultaneous optimization algorithm is applied to optimize both the process parameters and heat integration structures of the twocolumn configurations.The effectiveness of this approach is demonstrated through a case study focusing on industrial organosilicon separation.The results underscore that the superstructure methodology not only substantially mitigates computational time compared to exhaustive enumeration but also furnishes solutions that exhibit comparable performance.

Synthesis methods and powder quality of titanium monocarbide

Titanium monocarbide(TiC),which is the most stable titanium-based carbide,has attracted considerable interest in the fields of energy,catalysis,and structural materials due to its excellent properties.Synthesis of high-quality TiC powders with low cost and high efficiency is crucial for industrial applications;however major challenges face its realization.Herein,the methods for synthesizing TiC powders based on a reaction system are reviewed.This analysis is focused on the underlying mechanisms by which synthesis methods affect the quality of powders.Notably,strategies for improving the synthesis of highquality powders are analyzed from the perspective of enhancing heat and mass transfer processes.Furthermore,the critical issues,challenges,and development trends of the synthesis technology and application of high-quality TiC powder are discussed.

Microfluidic-oriented synthesis of enriched iridium nanodots/carbon architecture for robust electrocatalytic nitrogen fixation

Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless by-products.However,the chemical inertness of nitrogen and poor activated capacity on catalyst surface usually produce low ammonia yield and faradic efficiency.Herein,the microfluidic technology is proposed to efficiently fabricate enriched iridium nanodots/carbon architecture.Owing to in-situ co-precipitation reaction and microfluidic manipulation,the iridium nanodots/carbon nanomaterials possess small average size,uniform dispersion,high conductivity and abundant active sites,producing good proton activation and rapid electrons transmission and moderate adsorption/desorption capacity.As a result,the as-prepared iridium nanodots/carbon nanomaterials realize large ammonia yield of 28.73 μg h^(-1) cm^(-2) and faradic efficiency of 9.14%in KOH solution.Moreover,the high ammonia yield of 11.21 μg h^(-1) cm^(-2) and faradic efficiency of 24.30%are also achieved in H_(2)SO_(4) solution.The microfluidic method provides a reference for large-scale fabrication of nano-sized catalyst materials,which may accelerate the progress of electrocatalytic NRR in industrialization field.

运动干预对儿童执行功能影响的网状meta分析

目的:比较多种运动干预方案对儿童执行功能的影响。方法:检索中国知网、万方、pubmed、Web of science、Embase、Cochrane建库至2022年12月,关于运动干预对儿童执行功能影响的实验研究,采用Cochrane偏倚风险评估工具评估纳入文献质量,根据PICOS原则制定文献的纳入和排除标准,以标准化均数差(SMD)为效应指标。结果:纳入43篇文献(n=5 333)。Meta分析结果显示,促进儿童抑制控制首选单次运动时间≥51min、每周2次、干预周期≥17周的球类运动(SUCRA=86.8);促进儿童工作记忆首选单次运动时间10~30 min、每周2次、干预周期5~8周的球类运动(SUCRA=75.6);促进儿童认知灵活性首选单次运动时间31~50 min、每周2次、干预周期5~8周的球类运动(SUCRA=89.4)。结论:不同运动干预方案对儿童执行功能的影响效应不同。

Boosting Fischer-Tropsch Synthesis via Tuning of N Dopants in TiO_(2)@CN-Supported Ru Catalysts

Nitrogen(N)-doped carbon materials as metal catalyst supports have attracted signifi cant attention,but the eff ect of N dopants on catalytic performance remains unclear,especially for complex reaction processes such as Fischer-Tropsch synthesis(FTS).Herein,we engineered ruthenium(Ru)FTS catalysts supported on N-doped carbon overlayers on TiO_(2)nanoparticles.By regulating the carbonization temperatures,we successfully controlled the types and contents of N dopants to identify their impacts on metal-support interactions(MSI).Our fi ndings revealed that N dopants establish a favorable surface environment for electron transfer from the support to the Ru species.Moreover,pyridinic N demonstrates the highest electron-donating ability,followed by pyrrolic N and graphitic N.In addition to realizing excellent catalytic stability,strengthening the interaction between Ru sites and N dopants increases the Ru^(0)/Ru^(δ+)ratios to enlarge the active site numbers and surface electron density of Ru species to enhance the strength of adsorbed CO.Consequently,it improves the catalyst’s overall performance,encompassing intrinsic and apparent activities,as well as its ability for carbon chain growth.Accordingly,the as-synthesized Ru/TiO_(2)@CN-700 catalyst with abundant pyridine N dopants exhibits a superhigh C_(5+)time yield of 219.4 mol CO/(mol Ru·h)and C_(5+)selectivity of 85.5%.