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...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.展开更多
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 counterpart...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.展开更多
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 netw...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.展开更多
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...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.展开更多
Energetic materials,characterized by their capacity to store and release substantial energy,hold pivotal significance in some fields,particularly in defense applications.Microfluidics,with its ability to manipulate fl...Energetic materials,characterized by their capacity to store and release substantial energy,hold pivotal significance in some fields,particularly in defense applications.Microfluidics,with its ability to manipulate fluids and facilitate droplet formation at the microscale,enables precise control of chemical reactions.Recent scholarly endeavors have increasingly harnessed microfluidic reactors in the realm of energetic materials,yielding morphologically controllable particles with enhanced uniformity and explosive efficacy.However,crucial insights into microfluidic-based methodologies are dispersed across various publications,necessitating a systematic compilation.Accordingly,this review addresses this gap by concentrating on the synthesis of energetic materials through microfluidics.Specifically,the methods based on micro-mixing and droplets in the previous papers are summarized and the strategies to control the critical parameters within chemical reactions are discussed in detail.Then,the comparison in terms of advantages and disadvantages is attempted.As demonstrated in the last section regarding perspectives,challenges such as clogging,dead zones,and suboptimal production yields are non-ignoble in the promising fields and they might be addressed by integrating sound,optics,or electrical energy to meet heightened requirements.This comprehensive overview aims to consolidate and analyze the diverse array of microfluidic approaches in energetic material synthesis,offering valuable insights for future research directions.展开更多
Among hyperspectral imaging technologies, interferometric spectral imaging is widely used in remote sening due to advantages of large luminous flux and high resolution. However, with complicated mechanism, interferome...Among hyperspectral imaging technologies, interferometric spectral imaging is widely used in remote sening due to advantages of large luminous flux and high resolution. However, with complicated mechanism, interferometric imaging faces the impact of multi-stage degradation. Most exsiting interferometric spectrum reconstruction methods are based on tradition model-based framework with multiple steps, showing poor efficiency and restricted performance. Thus, we propose an interferometric spectrum reconstruction method based on degradation synthesis and deep learning.Firstly, based on imaging mechanism, we proposed an mathematical model of interferometric imaging to analyse the degradation components as noises and trends during imaging. The model consists of three stages, namely instrument degradation, sensing degradation, and signal-independent degradation process. Then, we designed calibration-based method to estimate parameters in the model, of which the results are used for synthesizing realistic dataset for learning-based algorithms.In addition, we proposed a dual-stage interferogram spectrum reconstruction framework, which supports pre-training and integration of denoising DNNs. Experiments exhibits the reliability of our degradation model and synthesized data, and the effectiveness of the proposed reconstruction method.展开更多
Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive st...Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented growth.The obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.展开更多
Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalit...Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalities.Among that,Cu nanoclusters have been gaining continuous increasing research attentions,thanks to the low cost,diversified structures,and superior catalytic performance for various reactions.In this review,we first summarize the recent progress regarding the synthetic methods of atomically precise Cu nanoclusters and the coordination modes between Cu and several typical ligands and then discuss the catalytic applications of these Cu nanoclusters with some explicit examples to explain the atomical-level structure-performance relationship.Finally,the current challenges and future research perspectives with some critical thoughts are elaborated.We hope this review can not only provide a whole picture of the current advances regarding the synthesis and catalytic applications of atomically precise Cu nanoclusters,but also points out some future research visions in this rapidly booming field.展开更多
Photocatalytic oxygen reduction for hydrogen peroxide(H_(2)O_(2))synthesis presents a green and costeffective production method.However,achieving highly selective H_(2)O_(2)synthesis remains challenging,necessitating ...Photocatalytic oxygen reduction for hydrogen peroxide(H_(2)O_(2))synthesis presents a green and costeffective production method.However,achieving highly selective H_(2)O_(2)synthesis remains challenging,necessitating precise control over free radical reaction pathways and minimizing undesirable oxidative by-products.Herein,we report for the visible light-driven simultaneous co-photocatalytic reduction of O2to H_(2)O_(2)and oxidation of biomass using the atomic rubidium-nitride modified carbon nitride(CNRb).The optimized CNRb catalyst demonstrates a record photoreduction rate of 8.01 mM h^(-1)for H_(2)O_(2)generation and photooxidation rate of 3.75 mM h^(-1)for furfuryl alcohol to furoic acid,achieving a remarkable solar-to-chemical conversion(SCC)efficiency of up to 2.27%.Experimental characterizations and DFT calculation disclosed that the introducing atomic Rb–N configurations allows for the high-selective generation of superoxide radicals while suppressing hydroxyl free radical formation.This is because the Rb–N serves as the new alternative site to perceive a stronger connection position for O2adsorption and reinforce the capability to extract protons,thereby triggering a high selective redox product formation.This study holds great potential in precisely regulating reactive radical processes at the atomic level,thereby paving the way for efficient synthesis of H_(2)O_(2)coupled with biomass valorization.展开更多
TiNb_(2)O_(7)has been emerged as one of the most promising electrode materials for high-energy lithium-ion batteries.However,limited by the slow electron/ion transport kinetics,and insufficient active sites in the bul...TiNb_(2)O_(7)has been emerged as one of the most promising electrode materials for high-energy lithium-ion batteries.However,limited by the slow electron/ion transport kinetics,and insufficient active sites in the bulk structure,the TiNb_(2)O_(7)electrode still suffers from unsatisfactory lithium storage performance.Herein,we demonstrate a spatially confined strategy toward a novel TiNb_(2)O_(7)-NMC/MXene composite through a triblock copolymer-directed one-pot solvothermal route,where TiNb_(2)O_(7)quantum dots with a particle size of 2-3 nm are evenly embedded into N-doped mesoporous carbon(NMC)and Ti_(3)C_(2)T_(X)MXene.Impressively,the as-prepared TiNb_(2)O_(7)-NMC/MXene anode exhibits a high reversible capacity(486.2 mAh g^(-1)at 0.1 A g^(-1)after 100 cycles)and long cycle lifespan(363.4 mAh g^(-1)at ss1 A g^(-1)after 500 cycles).Both experimental and theorical results further demonstrate that such a superior lithium storage performance is mainly ascribed to the synergistic effect among 0D TiNb_(2)O_(7)quantum dots,2D Ti_(3)C_(2)T_(X)MXene nanosheets,and N-doped mesoporous carbon.The strategy presented also opens up new horizon for space-confined preparation of high-performance electrode materials.展开更多
目的系统评价儿科体外膜肺氧合(ECMO)支持患者院内感染的流行病学特征。方法采用主题词与自由词相结合的方式,系统检索中国知网、万方医学数据库、中国生物医学文献数据库、维普数据库、Pubmed、Embase、web of science数据库,搜集关于...目的系统评价儿科体外膜肺氧合(ECMO)支持患者院内感染的流行病学特征。方法采用主题词与自由词相结合的方式,系统检索中国知网、万方医学数据库、中国生物医学文献数据库、维普数据库、Pubmed、Embase、web of science数据库,搜集关于儿科ECMO支持患者院内感染的观察性研究,检索时限均为建库到2023年12月。由2名研究者独立进行文献筛选、提取资料、评价纳入研究的偏倚风险后,使用Stata 18.0软件进行meta分析。结果共纳入16项研究,包括3353例儿科ECMO支持患者,其中发生院内感染患者712例。随机效应模型meta分析结果显示,院内感染发生率为28.55%[95%CI(22.26%,35.28%)]。病原学分布中以革兰阴性菌为主(约占68.68%),其中前3位为:鲍曼不动杆菌(26.93%)、肺炎克雷伯菌(11.90%)、铜绿假单胞菌(9.39%)。结论当前证据显示,儿科ECMO支持患者院内感染率较高,且可能受地域影响。受研究质量影响,上述结论尚待更高质量研究验证。展开更多
目的系统评价“乌头-半夏”反药配伍对大鼠的毒性。方法检索中国知网、万方数据、维普网、中国生物医学文献服务系统、PubMed、Embase和Web of Science数据库,纳入国内外已发表的关于反药“乌头-半夏”对大鼠毒性的研究,检索时限均从建...目的系统评价“乌头-半夏”反药配伍对大鼠的毒性。方法检索中国知网、万方数据、维普网、中国生物医学文献服务系统、PubMed、Embase和Web of Science数据库,纳入国内外已发表的关于反药“乌头-半夏”对大鼠毒性的研究,检索时限均从建库至2024年4月3日。由2名研究者独立筛选文献、提取资料并运用SYRCLE动物实验偏倚风险评估工具进行文献质量评价,采用RevMan 5.4软件进行Meta分析。结果最终纳入13篇文献。Meta分析结果显示,与空白对照组相比,乌头-半夏(1∶1)配伍对正常大鼠的肝脏指数、谷丙转氨酶(ALT)、肌酐(Cr)和尿素氮(BUN)无显著影响,但可显著升高正常大鼠的心脏指数、肾脏指数、谷草转氨酶(AST)、碱性磷酸酶(ALP)、肌酸激酶(CK)和肌酸激酶同工酶(CK-MB)含量;与乌头单用组相比,乌头-半夏(1∶1)配伍可降低正常大鼠的AST、ALP、CK含量和肾脏指数,但不能降低心脏指数和CK-MB含量。附子-半夏(1∶1)配伍与空白对照组相比,仅CK含量显著升高,但与缺血再灌注损伤模型大鼠相比,附子-半夏可逆转模型大鼠CK水平的变化。定性分析结果显示,乌头/附子-半夏配伍对正常大鼠心、肝、肾的组织病理无影响或有轻度损伤,附子-半夏配伍可改善心脏病理模型大鼠的心脏病理损伤。结论现有动物实验表明,乌头-半夏(1∶1)配伍对正常大鼠的肝脏、心脏、肾脏指标均有一定影响,但可减轻乌头单用对正常大鼠的肝、肾损伤,对乌头引起的心脏损伤影响较小。附子-半夏(1∶1)配伍对正常大鼠肝、肾指标无明显影响,对心脏指标有一定影响,但对心脏病理模型大鼠有一定的保护作用。因此,乌头-半夏反药临床应用仍需持有谨慎态度;附子-半夏在辩证准确、方药合理的前提下,或可取得良效。展开更多
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 recen...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.展开更多
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-...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.展开更多
目的:Meta分析钢板与外固定架固定治疗AO-C型桡骨远端骨折的临床疗效。方法:检索PubMed、Embase、Cochrane Library、Web of Science、中国知网、万方、维普和SinoMed数据库所有关于AO-C型桡骨远端骨折的随机对照临床试验的文献,检索时...目的:Meta分析钢板与外固定架固定治疗AO-C型桡骨远端骨折的临床疗效。方法:检索PubMed、Embase、Cochrane Library、Web of Science、中国知网、万方、维普和SinoMed数据库所有关于AO-C型桡骨远端骨折的随机对照临床试验的文献,检索时限均从各数据库建库到2023年6月30日。纳入研究参照Cochrane手册(Version6.3,2022)进行信息提取、文献质量评价,采用RevMan 5.4软件进行发表偏倚风险评价、检验异质性并进行Meta分析。结局指标为:影像学解剖指标(掌倾角、尺偏角、桡骨高度)、腕关节活动度(屈伸、旋转、尺桡偏)、并发症发生率、手术治疗情况比较(手术出血量、手术时间、住院时间、骨折愈合时间)和腕关节功能评分及相关量表。结果:(1)共纳入28项研究,患者共计2192例,包括1096例钢板内固定组和1096例外固定架组。(2)Meta分析结果显示:外固定架组的手术出血量[MD=-37.93,95%CI(-48.54,-27.31),P<0.00001]、手术时间[MD=-31.58,95%CI(-48.96,-14.20),P=0.0004]、住院时间[MD=-4.58,95%CI(-5.44,-3.71),P<0.00001]、骨折愈合时间[MD=-0.88,95%CI(-1.35,-0.41),P=0.0002]均显著优于钢板内固定组(P<0.05)。(3)两组的掌倾角[MD=-0.17,95%CI(-0.95,0.61),P=0.68]、尺偏角[MD=0.22,95%CI(-0.73,1.17),P=0.65]、桡骨高度[MD=-0.24,95%CI(-1.15,0.67),P=0.60],屈伸[MD=-5.63,95%CI(-11.85,0.58),P=0.08]、旋转[MD=-5.80,95%CI(-12.77,1.17),P=0.10]、尺桡偏[MD=-2.86,95%CI(-10.87,5.15),P=0.48],并发症发生率[RR=0.96,95%CI(0.63,1.46),P=0.83],Gartland-Werley腕部临床评分[MD=0.13,95%CI(-0.80,1.06),P=0.78]、Gartland-Werley腕部临床评分优良率[RR=0.93,95%CI(0.87,1.01),P=0.08]、Cooney腕关节评分优良率[RR=0.99,95%CI(0.62,1.59),P=0.98]、腕关节DASH评分[MD=-4.67,95%CI(-14.96,5.62),P=0.37]的差异均无统计学意义(P>0.05)。结论:与钢板内固定相比,外固定架治疗AO-C型桡骨远端骨折可以显著减少手术出血量、缩短手术时间与住院时间和骨折愈合时间,其影像学解剖指标、腕关节活动度、并发症发生率和腕关节功能评分两者相当。展开更多
基金the support from the CIPHER Project(IIID 2018-008)funded by the Commission on Higher Education-Philippine California Advanced Research Institutes(CHED-PCARI)。
文摘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.
基金supported by the Teli Fellowship from Beijing Institute of Technology,the National Natural Science Foundation of China(Nos.52303366,22173109).
文摘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.
基金The authors are grateful for the financial support from National Natural Science Foundation of China(32001728).
文摘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.
基金financially supported by the National Natural Science Foundation of China(21975100).
文摘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.
基金financially supported by Science and Technology on Applied Physical Chemistry Laboratory,China(Grant No.61426022220303)supported by the Young Scientists Fund of the National Natural Science Foundation of China(Grant No.52305617)。
文摘Energetic materials,characterized by their capacity to store and release substantial energy,hold pivotal significance in some fields,particularly in defense applications.Microfluidics,with its ability to manipulate fluids and facilitate droplet formation at the microscale,enables precise control of chemical reactions.Recent scholarly endeavors have increasingly harnessed microfluidic reactors in the realm of energetic materials,yielding morphologically controllable particles with enhanced uniformity and explosive efficacy.However,crucial insights into microfluidic-based methodologies are dispersed across various publications,necessitating a systematic compilation.Accordingly,this review addresses this gap by concentrating on the synthesis of energetic materials through microfluidics.Specifically,the methods based on micro-mixing and droplets in the previous papers are summarized and the strategies to control the critical parameters within chemical reactions are discussed in detail.Then,the comparison in terms of advantages and disadvantages is attempted.As demonstrated in the last section regarding perspectives,challenges such as clogging,dead zones,and suboptimal production yields are non-ignoble in the promising fields and they might be addressed by integrating sound,optics,or electrical energy to meet heightened requirements.This comprehensive overview aims to consolidate and analyze the diverse array of microfluidic approaches in energetic material synthesis,offering valuable insights for future research directions.
文摘Among hyperspectral imaging technologies, interferometric spectral imaging is widely used in remote sening due to advantages of large luminous flux and high resolution. However, with complicated mechanism, interferometric imaging faces the impact of multi-stage degradation. Most exsiting interferometric spectrum reconstruction methods are based on tradition model-based framework with multiple steps, showing poor efficiency and restricted performance. Thus, we propose an interferometric spectrum reconstruction method based on degradation synthesis and deep learning.Firstly, based on imaging mechanism, we proposed an mathematical model of interferometric imaging to analyse the degradation components as noises and trends during imaging. The model consists of three stages, namely instrument degradation, sensing degradation, and signal-independent degradation process. Then, we designed calibration-based method to estimate parameters in the model, of which the results are used for synthesizing realistic dataset for learning-based algorithms.In addition, we proposed a dual-stage interferogram spectrum reconstruction framework, which supports pre-training and integration of denoising DNNs. Experiments exhibits the reliability of our degradation model and synthesized data, and the effectiveness of the proposed reconstruction method.
基金Joint Project of Dalian University of Technology-Dalian Institute of Chemical Physics (HX20230236)。
文摘Zeolite nanosheets with a short b-axis thickness are highly desirable in lots of catalytic reactions due to their reduced diffusion resistance. Nevertheless, conventional synthesis methods usually require expensive structure-directing agents(SDAs), pricey raw materials, and eco-unfriendly fluorine-containing additives. Here, we contributed a cost-effective and fluoride-free synthesis method for synthesizing high-quality MFI zeolite nanosheets through a Silicalite-1(Sil-1) seed suspension and urea cooperative strategy, only with inexpensive colloidal silica as the Si source. Our approach was effective for synthesizing both Sil-1 and aluminum-containing ZSM-5 nanosheets. By optimizing key synthesis parameters,including seed aging time, seed quantity, and urea concentration, we achieved precise control over the crystal face aspect ratio and b-axis thickness. We also revealed a non-classical oriented nanosheet growth mechanism, where Sil-1 seeds induced the formation of quasi-ordered precursor particles, and the(010)crystal planes of these particles facilitated urea adsorption, thereby promoting c-axis-oriented growth.The obtained ZSM-5 nanosheets exhibited exceptional catalytic performance in the benzene alkylation with ethanol, maintaining stability for over 500 h, which is 5 times longer than traditional ZSM-5 catalysts. Furthermore, large-scale production of ZSM-5 nanosheets was successfully carried out in a 3 L highpressure autoclave, yielding samples consistent with those from laboratory-scale synthesis. This work marks a significant step forward in the sustainable and efficient production of MFI nanosheets using inexpensive and environmentally friendly raw materials, offering the broad applicability in catalysis.
基金supported by the open funds of Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University), Ministry of Education, Chinathe funding from Guangdong Natural Science Funds (No. 2023A0505050107)。
文摘Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalities.Among that,Cu nanoclusters have been gaining continuous increasing research attentions,thanks to the low cost,diversified structures,and superior catalytic performance for various reactions.In this review,we first summarize the recent progress regarding the synthetic methods of atomically precise Cu nanoclusters and the coordination modes between Cu and several typical ligands and then discuss the catalytic applications of these Cu nanoclusters with some explicit examples to explain the atomical-level structure-performance relationship.Finally,the current challenges and future research perspectives with some critical thoughts are elaborated.We hope this review can not only provide a whole picture of the current advances regarding the synthesis and catalytic applications of atomically precise Cu nanoclusters,but also points out some future research visions in this rapidly booming field.
基金National Natural Science Foundation of China(22309032,22109120,and 62104170)Guangdong Basic and Applied Basic Research Foundation(2022A1515011737)+2 种基金Science and Technology Program of Guangzhou(2023A04J1395)GDAS’Project of Science and Technology Development(2021GDASYL-20210102010)Zhejiang Provincial Natural Science Foundation of China(LY23F040001)。
文摘Photocatalytic oxygen reduction for hydrogen peroxide(H_(2)O_(2))synthesis presents a green and costeffective production method.However,achieving highly selective H_(2)O_(2)synthesis remains challenging,necessitating precise control over free radical reaction pathways and minimizing undesirable oxidative by-products.Herein,we report for the visible light-driven simultaneous co-photocatalytic reduction of O2to H_(2)O_(2)and oxidation of biomass using the atomic rubidium-nitride modified carbon nitride(CNRb).The optimized CNRb catalyst demonstrates a record photoreduction rate of 8.01 mM h^(-1)for H_(2)O_(2)generation and photooxidation rate of 3.75 mM h^(-1)for furfuryl alcohol to furoic acid,achieving a remarkable solar-to-chemical conversion(SCC)efficiency of up to 2.27%.Experimental characterizations and DFT calculation disclosed that the introducing atomic Rb–N configurations allows for the high-selective generation of superoxide radicals while suppressing hydroxyl free radical formation.This is because the Rb–N serves as the new alternative site to perceive a stronger connection position for O2adsorption and reinforce the capability to extract protons,thereby triggering a high selective redox product formation.This study holds great potential in precisely regulating reactive radical processes at the atomic level,thereby paving the way for efficient synthesis of H_(2)O_(2)coupled with biomass valorization.
基金support from the Natural Science Foundation of Shanghai(23ZR1423800),Shuguang Program supported by Shanghai Education Development Foundation and Shanghai Municipal Education Commission(18SG35)Open Research Fund of Shanghai Key Laboratory of Green Chemistry and Chemical Processes(East China Normal University)Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University.
文摘TiNb_(2)O_(7)has been emerged as one of the most promising electrode materials for high-energy lithium-ion batteries.However,limited by the slow electron/ion transport kinetics,and insufficient active sites in the bulk structure,the TiNb_(2)O_(7)electrode still suffers from unsatisfactory lithium storage performance.Herein,we demonstrate a spatially confined strategy toward a novel TiNb_(2)O_(7)-NMC/MXene composite through a triblock copolymer-directed one-pot solvothermal route,where TiNb_(2)O_(7)quantum dots with a particle size of 2-3 nm are evenly embedded into N-doped mesoporous carbon(NMC)and Ti_(3)C_(2)T_(X)MXene.Impressively,the as-prepared TiNb_(2)O_(7)-NMC/MXene anode exhibits a high reversible capacity(486.2 mAh g^(-1)at 0.1 A g^(-1)after 100 cycles)and long cycle lifespan(363.4 mAh g^(-1)at ss1 A g^(-1)after 500 cycles).Both experimental and theorical results further demonstrate that such a superior lithium storage performance is mainly ascribed to the synergistic effect among 0D TiNb_(2)O_(7)quantum dots,2D Ti_(3)C_(2)T_(X)MXene nanosheets,and N-doped mesoporous carbon.The strategy presented also opens up new horizon for space-confined preparation of high-performance electrode materials.
文摘目的系统评价儿科体外膜肺氧合(ECMO)支持患者院内感染的流行病学特征。方法采用主题词与自由词相结合的方式,系统检索中国知网、万方医学数据库、中国生物医学文献数据库、维普数据库、Pubmed、Embase、web of science数据库,搜集关于儿科ECMO支持患者院内感染的观察性研究,检索时限均为建库到2023年12月。由2名研究者独立进行文献筛选、提取资料、评价纳入研究的偏倚风险后,使用Stata 18.0软件进行meta分析。结果共纳入16项研究,包括3353例儿科ECMO支持患者,其中发生院内感染患者712例。随机效应模型meta分析结果显示,院内感染发生率为28.55%[95%CI(22.26%,35.28%)]。病原学分布中以革兰阴性菌为主(约占68.68%),其中前3位为:鲍曼不动杆菌(26.93%)、肺炎克雷伯菌(11.90%)、铜绿假单胞菌(9.39%)。结论当前证据显示,儿科ECMO支持患者院内感染率较高,且可能受地域影响。受研究质量影响,上述结论尚待更高质量研究验证。
文摘目的系统评价“乌头-半夏”反药配伍对大鼠的毒性。方法检索中国知网、万方数据、维普网、中国生物医学文献服务系统、PubMed、Embase和Web of Science数据库,纳入国内外已发表的关于反药“乌头-半夏”对大鼠毒性的研究,检索时限均从建库至2024年4月3日。由2名研究者独立筛选文献、提取资料并运用SYRCLE动物实验偏倚风险评估工具进行文献质量评价,采用RevMan 5.4软件进行Meta分析。结果最终纳入13篇文献。Meta分析结果显示,与空白对照组相比,乌头-半夏(1∶1)配伍对正常大鼠的肝脏指数、谷丙转氨酶(ALT)、肌酐(Cr)和尿素氮(BUN)无显著影响,但可显著升高正常大鼠的心脏指数、肾脏指数、谷草转氨酶(AST)、碱性磷酸酶(ALP)、肌酸激酶(CK)和肌酸激酶同工酶(CK-MB)含量;与乌头单用组相比,乌头-半夏(1∶1)配伍可降低正常大鼠的AST、ALP、CK含量和肾脏指数,但不能降低心脏指数和CK-MB含量。附子-半夏(1∶1)配伍与空白对照组相比,仅CK含量显著升高,但与缺血再灌注损伤模型大鼠相比,附子-半夏可逆转模型大鼠CK水平的变化。定性分析结果显示,乌头/附子-半夏配伍对正常大鼠心、肝、肾的组织病理无影响或有轻度损伤,附子-半夏配伍可改善心脏病理模型大鼠的心脏病理损伤。结论现有动物实验表明,乌头-半夏(1∶1)配伍对正常大鼠的肝脏、心脏、肾脏指标均有一定影响,但可减轻乌头单用对正常大鼠的肝、肾损伤,对乌头引起的心脏损伤影响较小。附子-半夏(1∶1)配伍对正常大鼠肝、肾指标无明显影响,对心脏指标有一定影响,但对心脏病理模型大鼠有一定的保护作用。因此,乌头-半夏反药临床应用仍需持有谨慎态度;附子-半夏在辩证准确、方药合理的前提下,或可取得良效。
基金support from the National Key Research and Development Program of China(2021YFA1500401,2021YFA1501202)the National Natural Science Foundation of China(22288101)the 111 Project(B17020)for supporting this work.
文摘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.
基金supported by the National Natural Science Foundation of China(22025801)and(22208190)National Postdoctoral Program for Innovative Talents(BX2021146)Shuimu Tsinghua Scholar Program(2021SM055).
文摘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.
文摘目的:Meta分析钢板与外固定架固定治疗AO-C型桡骨远端骨折的临床疗效。方法:检索PubMed、Embase、Cochrane Library、Web of Science、中国知网、万方、维普和SinoMed数据库所有关于AO-C型桡骨远端骨折的随机对照临床试验的文献,检索时限均从各数据库建库到2023年6月30日。纳入研究参照Cochrane手册(Version6.3,2022)进行信息提取、文献质量评价,采用RevMan 5.4软件进行发表偏倚风险评价、检验异质性并进行Meta分析。结局指标为:影像学解剖指标(掌倾角、尺偏角、桡骨高度)、腕关节活动度(屈伸、旋转、尺桡偏)、并发症发生率、手术治疗情况比较(手术出血量、手术时间、住院时间、骨折愈合时间)和腕关节功能评分及相关量表。结果:(1)共纳入28项研究,患者共计2192例,包括1096例钢板内固定组和1096例外固定架组。(2)Meta分析结果显示:外固定架组的手术出血量[MD=-37.93,95%CI(-48.54,-27.31),P<0.00001]、手术时间[MD=-31.58,95%CI(-48.96,-14.20),P=0.0004]、住院时间[MD=-4.58,95%CI(-5.44,-3.71),P<0.00001]、骨折愈合时间[MD=-0.88,95%CI(-1.35,-0.41),P=0.0002]均显著优于钢板内固定组(P<0.05)。(3)两组的掌倾角[MD=-0.17,95%CI(-0.95,0.61),P=0.68]、尺偏角[MD=0.22,95%CI(-0.73,1.17),P=0.65]、桡骨高度[MD=-0.24,95%CI(-1.15,0.67),P=0.60],屈伸[MD=-5.63,95%CI(-11.85,0.58),P=0.08]、旋转[MD=-5.80,95%CI(-12.77,1.17),P=0.10]、尺桡偏[MD=-2.86,95%CI(-10.87,5.15),P=0.48],并发症发生率[RR=0.96,95%CI(0.63,1.46),P=0.83],Gartland-Werley腕部临床评分[MD=0.13,95%CI(-0.80,1.06),P=0.78]、Gartland-Werley腕部临床评分优良率[RR=0.93,95%CI(0.87,1.01),P=0.08]、Cooney腕关节评分优良率[RR=0.99,95%CI(0.62,1.59),P=0.98]、腕关节DASH评分[MD=-4.67,95%CI(-14.96,5.62),P=0.37]的差异均无统计学意义(P>0.05)。结论:与钢板内固定相比,外固定架治疗AO-C型桡骨远端骨折可以显著减少手术出血量、缩短手术时间与住院时间和骨折愈合时间,其影像学解剖指标、腕关节活动度、并发症发生率和腕关节功能评分两者相当。
