Palladium(Pd)has long been constrained as a potential catalyst for CO2reduction reactions(CO2RR)due to significant deactivation caused by strongly adsorbed carbonaceous intermediates on its surface,severely limi...Palladium(Pd)has long been constrained as a potential catalyst for CO2reduction reactions(CO2RR)due to significant deactivation caused by strongly adsorbed carbonaceous intermediates on its surface,severely limiting its catalytic activity and stability.To address this critical bottleneck,this study proposes and implements a synergistic regulation strategy combining alloying and spatial confinement effects.This approach designs a composite catalyst by encapsulating boron-silver co-doped palladium alloy nanoparticles(B-Ag4Pd6)within hollow porous resin carbon spheres(HPRCS).In an H-cell,this catalyst achieved a CO Faradaic efficiency of 96.19%at jCO=24.8 mA/cm2 and maintained stable performance for 80 h.Even under flow cell conditions,it sustained 91.23%CO selectivity at jCO=157.86 mA/cm2 over 60 h.Experimental comparisons confirmed the significant promoting effect of spatial confinement on CO2RR.Furthermore,in situ ATR-FTIR spectroscopy and density functional theory(DFT)calculations reveal that B/Ag alloying downshifts the Pd d-band center,optimizes(*)^COOH and(*)^CO adsorption,and the confined Hmicroenvironment accelerates CO formation while suppressing hydrogen evolution.This study not only successfully addressed the issue of carbon intermediate poisoning on Pd surfaces through alloying and microenvironmental regulation,but also provides novel insights and approaches for designing high-performance CO2RR catalysts that integrate electronic structure control with microenvironmental engineering.展开更多
Pulsating flow is a common condition for under water manipulators in Bohai Bay.This study aimed to investigate the effects of pulsation frequency and amplitude on the hydrodynamic characteristics of an underwater mani...Pulsating flow is a common condition for under water manipulators in Bohai Bay.This study aimed to investigate the effects of pulsation frequency and amplitude on the hydrodynamic characteristics of an underwater manipulator with different postures using the user-defined function (UDF) method. The lift coefficient (CL), drag coefficient (CD), and vortex shedding of the underwater manipulator in single-and dualarm forms were obtained. Results indicated that the maximum increase in the lift and drag coefficients subjected to the pulsation parameters was 24.45%and 28%, respectively, when the fluid flowed past a single arm. Compared with the single arm, the lift and drag coefficients of the arms were higher than those of the single arm when arm 2 was located upstream. Additionally, the pulsation frequency had no obvious effect on the manipulator, but the CL and CD of arm 2 showed an obvious increasing trend with an increase in pulsation amplitude. Meanwhile, when arm 2 was located downstream, the CL and CD of arm 2 were reduced by 16.38%and 1.15%, respectively, with an increase in the pulse frequency,and the maximum increase in the lift and dragcoefficients was 33.33%and 16.78%,respectively,with increasing pulsation amplitude.Moreover, the downstream wake morphology changed significantly, and a combined vortex phenomenon appeared. Finally, a theoretical basis for examining the hydrodynamic characteristics of marine engineering equipment was established to aid future marine resource exploitation.展开更多
Environmental factors significantly affected the succession of microbial communities during the fermentation of Huangjiu Raw wheat Qu(RWQ).Influence of environmental factors on microbial community during fermentation ...Environmental factors significantly affected the succession of microbial communities during the fermentation of Huangjiu Raw wheat Qu(RWQ).Influence of environmental factors on microbial community during fermentation of Chinese Huangjiu RWQ.The interaction of environmental factors and microorganisms affects the changes of microbial communities and key enzyme transcript levels in different stages during the production of Huangjiu RWQ.This study combined environmental factor analysis and high-throughput sequencing technology to comprehensively analyze the specific changes of microbial communities and environmental factors at each stage of Huangjiu production.In addition,the influence of the interaction of environmental factors and microorganisms on microbial succession was investigated by correlation analysis,and the enzymes related to saccharification and ethanol fermentation during the production of RWQ were explored.The results showed that Bacillus,Weisseria,Thermophilic actinomycetes and Lactobacillus were the dominant bacteria in RWQ,while Aspergillus,Thermomyces,Fusarium and Alternaria were the dominant fungi.Fungi were active in the early stage of RWQ fermentation,while bacteria were active in the middle and late stage of fermentation.Microbial community succession was closely related to environmental humidity and CO2.These environmental factors were positively correlated with most fungi,but negatively correlated with Thermophilic actinomycetes,Glycopolyspora and Acinetobacter.In fungi,the enzymes related to saccharification and fermentation mainly came from Thermophilic ascomycetes and thermophilic fungi,while in Bacteria,these two enzymes mainly came from weisseria.This study revealed the relationship between RWQ microbe and environmental factors,which was helpful to clarify the succession law of RWQ microbe.展开更多
基金financial support from the National Natural Science Foundation of China(72088101,22474157)the Major Program from Xiangjiang Laboratory(23XJ01010,23XJ01011)+2 种基金the Natural Science Foundation of Hunan Province(2024JJ5417)the Innovation-Driven Project of Central South University(2023CXQD048)the Changsha Natural Science Foundation Project(kq2402199)。
摘要Palladium(Pd)has long been constrained as a potential catalyst for CO2reduction reactions(CO2RR)due to significant deactivation caused by strongly adsorbed carbonaceous intermediates on its surface,severely limiting its catalytic activity and stability.To address this critical bottleneck,this study proposes and implements a synergistic regulation strategy combining alloying and spatial confinement effects.This approach designs a composite catalyst by encapsulating boron-silver co-doped palladium alloy nanoparticles(B-Ag4Pd6)within hollow porous resin carbon spheres(HPRCS).In an H-cell,this catalyst achieved a CO Faradaic efficiency of 96.19%at jCO=24.8 mA/cm2 and maintained stable performance for 80 h.Even under flow cell conditions,it sustained 91.23%CO selectivity at jCO=157.86 mA/cm2 over 60 h.Experimental comparisons confirmed the significant promoting effect of spatial confinement on CO2RR.Furthermore,in situ ATR-FTIR spectroscopy and density functional theory(DFT)calculations reveal that B/Ag alloying downshifts the Pd d-band center,optimizes(*)^COOH and(*)^CO adsorption,and the confined Hmicroenvironment accelerates CO formation while suppressing hydrogen evolution.This study not only successfully addressed the issue of carbon intermediate poisoning on Pd surfaces through alloying and microenvironmental regulation,but also provides novel insights and approaches for designing high-performance CO2RR catalysts that integrate electronic structure control with microenvironmental engineering.
基金the National Natural Science Foundation of China (No. 51905211)China Postdoctoral Science Foundation (Grant No. 2020M672128)+1 种基金University of Jinan Research Startup and Discipline Construction Fund (Grant No.1009435)a Project of the “20 Regulations for New Universities” funding program of Jinan (No.202228116)。
摘要Pulsating flow is a common condition for under water manipulators in Bohai Bay.This study aimed to investigate the effects of pulsation frequency and amplitude on the hydrodynamic characteristics of an underwater manipulator with different postures using the user-defined function (UDF) method. The lift coefficient (CL), drag coefficient (CD), and vortex shedding of the underwater manipulator in single-and dualarm forms were obtained. Results indicated that the maximum increase in the lift and drag coefficients subjected to the pulsation parameters was 24.45%and 28%, respectively, when the fluid flowed past a single arm. Compared with the single arm, the lift and drag coefficients of the arms were higher than those of the single arm when arm 2 was located upstream. Additionally, the pulsation frequency had no obvious effect on the manipulator, but the CL and CD of arm 2 showed an obvious increasing trend with an increase in pulsation amplitude. Meanwhile, when arm 2 was located downstream, the CL and CD of arm 2 were reduced by 16.38%and 1.15%, respectively, with an increase in the pulse frequency,and the maximum increase in the lift and dragcoefficients was 33.33%and 16.78%,respectively,with increasing pulsation amplitude.Moreover, the downstream wake morphology changed significantly, and a combined vortex phenomenon appeared. Finally, a theoretical basis for examining the hydrodynamic characteristics of marine engineering equipment was established to aid future marine resource exploitation.
基金supported by the Foundation of Public Projects of Zhejiang Province,China(No.LGN22C200008)The Zhejiang Shaoxing Huangjiu Industry Innovation Service Complex-Technological Innovation Project in Zhejiang Province(No.2023KJ082)+4 种基金Jiangsu Province Innovation and Entrepreneurship Program(JSSCRC2021569)Program Foundation of Public Projects of Shaoxing city,Zhejiang Province,China(No.2018C30010)Foundation of Public Projects of Zhejiang Province,China(No.2017C32101)Shaoxing University Fund(No.08021066)Shaoxing University Fund(No.08220102213).
摘要Environmental factors significantly affected the succession of microbial communities during the fermentation of Huangjiu Raw wheat Qu(RWQ).Influence of environmental factors on microbial community during fermentation of Chinese Huangjiu RWQ.The interaction of environmental factors and microorganisms affects the changes of microbial communities and key enzyme transcript levels in different stages during the production of Huangjiu RWQ.This study combined environmental factor analysis and high-throughput sequencing technology to comprehensively analyze the specific changes of microbial communities and environmental factors at each stage of Huangjiu production.In addition,the influence of the interaction of environmental factors and microorganisms on microbial succession was investigated by correlation analysis,and the enzymes related to saccharification and ethanol fermentation during the production of RWQ were explored.The results showed that Bacillus,Weisseria,Thermophilic actinomycetes and Lactobacillus were the dominant bacteria in RWQ,while Aspergillus,Thermomyces,Fusarium and Alternaria were the dominant fungi.Fungi were active in the early stage of RWQ fermentation,while bacteria were active in the middle and late stage of fermentation.Microbial community succession was closely related to environmental humidity and CO2.These environmental factors were positively correlated with most fungi,but negatively correlated with Thermophilic actinomycetes,Glycopolyspora and Acinetobacter.In fungi,the enzymes related to saccharification and fermentation mainly came from Thermophilic ascomycetes and thermophilic fungi,while in Bacteria,these two enzymes mainly came from weisseria.This study revealed the relationship between RWQ microbe and environmental factors,which was helpful to clarify the succession law of RWQ microbe.