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Modified electronic structure and enhanced hydroxyl adsorption make quaternary Pt-based nanosheets efficient anode electrocatalysts for formic acid-/alcohol-air fuel cells

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Journal of Energy Chemistry 2024年第5期92卷 142-150页

作者： Fengling Zhao Qiang Yuan siyang nie Liang Wu Xun Wang State-Local Joint Laboratory for Comprehensive Utilization of Biomass Center for R&D of Fine ChemicalsCollege of Chemistry and Chemical EngineeringGuizhou UniversityGuiyang 550025GuizhouChina Key Lab of Organic Optoelectronics&Molecular Engineering Tsinghua UniversityBeijing 100084China School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China

Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)ultrathin nanosheets is fabricated and used as high-performance anode electrocatalysts for formic acid-/alcohol-air fuel cells.The modified electronic structure of Pt,enhanced hydroxyl adsorption,and abundant exterior defects afford Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C high intrinsic anodic electrocatalytic activity to boost the power densities of direct formic acid-/methanol-/ethanol-/ethylene glycol-/glycerol-air fuel cells,and the corresponding peak power density of Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C is respectively 129.7,142.3,105.4,124.3,and 128.0 mW cm^(-2),considerably outperforming Pt/C.Operando in situ Fourier transform infrared reflection spectroscopy reveals that formic acid oxidation on Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)/C occurs via a CO_(2)-free direct pathway.Density functional theory calculations show that the presence of Ag,Bi,and Te in Pt_(1)Ag_(0.1)Bi_(0.16)Te_(0.29)suppresses CO^(*)formation while optimizing dehydrogenation steps and synergistic effect and modified Pt effectively enhance H_(2)O dissociation to improve electrocatalytic performance.This synthesis strategy can be extended to 43 other types of ultrathin multimetallic nanosheets(from ternary to octonary nanosheets),and efficiently capture precious metals(i.e.,Pd,Pt,Rh,Ru,Au,and Ag)from different water sources.

关键词： Pt-based nanosheets Modifiedelectronic structure Enhanced hydroxyl adsorption Formicacidand alcohol oxidation Direct liquid fuel cells

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Enthalpy-change driven synthesis of high-entropy perovskite nanoparticles

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Nano Research 2022年第6期15卷 4867-4872页

作者： siyang nie Liang Wu Lingci Zhao Pengfei Zhang School of Chemistry and Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China

Due to their diverse and tunable composition,distorted lattice and excellent stability,high-entropy ceramics(HECs)hold great promise for catalysis,especially when they present as nanoparticles(NPs).However,current HECs are typically limited to bulky materials with none or fewer defects,because high synthetic temperature(e.g.,1,000–1,200°C)is usually required to highlight the entropic contribution(TΔS)inΔG=ΔH−TΔS.Being different with previous strategies,a negative Gibbs free energy for HECs crystallization is obtained by dramatically decreasing the mixing enthalpy(ΔH).Guided by this principle,single-phase highentropy La(Ni_(0.2)Mn_(0.2)Cu_(0.2)Fe_(0.2)Co_(0.2))O_(3−δ)perovskite(HE-LMO)NPs were prepared at a relatively low temperature(≤500°C).Interestingly,abundant oxygen vacancies were directly created within HE-LMO NPs,which exhibited good activity in catalytic oxidation.Meanwhile,the high-entropy structure endows as-made HE-LMO with robust stability even with 5 vol.%water in feeding gas.Density functional theory(DFT)calculations revealed that the defective sites in HE-LMO NPs facilitated the charge transfer from HE-LMO to CO,thus activating the adsorbed CO gas.The current work may inspire future design and synthesis of HECs NPs.

关键词： enthalpy-change high-entropy ceramics mechanochemical synthesis perovskite CO oxidation

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Ultrathin zirconium-porphyrin based nanobelts as photo-coupled electrocatalysis for CH_(4) oxidation to CO

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Nano Research 2023年第11期16卷 12641-12646页

作者： Haoming Guo Liang Wu siyang nie Deren Yang Xun Wang Key Lab of Organic Optoelectronics and Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084China Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China Institute of Energy Power Innovation North China Electric Power UniversityBeijing 102206China

The development of novel and effective methods for the activation of methane is fascinating,which offers a promising potential for the sustainable development of chemical industry and the mitigation of greenhouse effect.Here we successfully synthesize two-dimensional(2D)Zr/5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin(TCPP)ultrathin nanobelts(UNBs)as a high efficiency catalyst for methane(CH_(4))oxidation to carbon monoxide(CO).The Co-UNBs show well photo-coupled electrocatalytic performances for CH4 activation(CO production rates are 0.171 and 8.416 mmol·g−1·h−1 under dark/visible light,respectively).Density functional theory(DFT)calculations were performed to illustrate the mechanism of photoelectrocatalytic process and the high efficiency oxidation of CH4 to CO.Based on the ultrathin structure and highly efficient catalytic properties,this work provides a prospecting avenue for the design and synthesis of methane oxidation catalyst.

关键词： ultrathin Co-Zr/5 10 15 20-tetrakis(4-carboxyphenyl)porphyrin(TCPP)nanobelts photo-coupled electrocatalyst CH_(4)oxidation density functional theory(DFT)calculation

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Comprehensive insights:unraveling the mechanisms of gut commensals in glucose metabolism regulation

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Science China(Life Sciences) 2024年第2期67卷 414-417页

作者： Zhipeng Li Qixing nie Shao-Ping nie State Key Laboratory of Food Science and Resources China-Canada Joint Lab of Food Science and Technology(Nanchang)Key Laboratory of Bioactive Polysaccharides of Jiangxi ProvinceNanchang UniversityNanchang 330047China

The prevalence of type 2 diabetes(T2D)has escalated to a global epidemic,garnering widespread concern.Tremendous research utilizing germ-free(GF)mice,antibiotic treatments,and fecal microbiota transplantation approaches has established the critical role of gut microbiota in modulating glucose metabolism.The microbiota interacts with diets and the mucosal immune system,influencing intestinal permeability and the penetration of microbial products.

关键词： metabolism utilizing insight

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The Role of Childhood Circumstances in Healthy Aging Inequalities Among Older Adults—China,2011–2020

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China CDC weekly 2024年第11期6卷 208-212,I0004-I0007页

作者： Peng nie Xili Lin Lanlin Ding School of Economics and Finance Xi’an Jiaotong UniversityXi’an CityShaanxi ProvinceChina Global Health Institute Xi’an Jiaotong University Health Science CenterXi’an CityShaanxi ProvinceChina National School of Development Peking UniversityBeijingChina

What is already known about this topic?Addressing health disparities is a worldwide priority,with a well-established acknowledgment of the influence of childhood circumstances on these discrepancies.In China,particularly among the elderly,health inequalities are a notable concern.What is added by this report?The inequality in healthy aging has increased from 2011 to 2020,both in general and concerning childhood factors.Nevertheless,the impact of early-life healthcare access and parental health behaviors on healthy aging gaps has reduced among older adults in better health within the top segment of healthy aging.What are the implications for public health practice?Efforts towards reducing regional health disparities and improving healthcare access for children,along with promoting the health and well-being of parents,especially in economically disadvantaged households,are crucial policy considerations.

关键词： ledgment inequalities circumstances

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Recent advances in small-scale hydrogel-based robots for adaptive biomedical applications

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Nano Research 2024年第2期17卷 649-662页

作者： Mingzhe nie Qilong Zhao Xuemin Du Institute of Biomedical&Health Engineering Shenzhen Institute of Advanced Technology(SIAT)Chinese Academy of Sciences(CAS)Shenzhen 518055China

Small-scale robots,ranging in size from micrometers to centimeters,have gained significant attention in the biomedical field.However,conventional small-scale robots made of rigid materials encounter challenges in adapting themselves to the soft tissues and complicated environments of human body.Compared to the rigid counterpart,small-scale hydrogel-based robots hold great promises due to their tissue-like low modulus,outstanding biocompatibility and accessible stimuli-responsive capabilities.These attributes offer small-scale hydrogel-based robots with multimodal locomotion and reinforced functions,further enhancing the adaptability in manipulation and tasks execution for various biomedical applications.In this review,we present recent advances in small-scale hydrogel-based robots.We first summarize the design principles of small-scale hydrogel-based robots including materials,fabrication techniques and manipulation strategies,then highlighting their upgraded functions and adaptive biomedical applications.Finally,we discuss existing challenges and future perspectives for small-scale hydrogel-based robots.

关键词： small-scale robot hydrogel locomotion multi-function adaptability

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Matched Volterra reduced-order model for an airfoil undergoing periodic translation

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Chinese Journal of Aeronautics 2024年第1期37卷 19-23页

作者： Lianrui nie Ziniu WU Department of Engineering Mechanics Tsinghua UniversityBeijing 100084China

This paper is devoted to application of the Reduced-Order Model(ROM)based on Volterra series to prediction of lift and drag forces due to airfoil periodic translation in transonic flow region.When there is large amplitude oscillation of the relative Mach number,as appeared in helicopter rotor movement in forward flight,the conventional Volterra ROM is found to be unsatisfactory.To cover such applications,a matched Volterra ROM,inspired from previous multistep nonlinear indicial response method based on Duhamel integration,is thus considered,in which the step motions are defined inside a number of equal intervals with both positive and negative step motions to match the airfoil forward and backward movement,and the kernel functions are constructed independently at each interval.It shows that,at least for the translation movement considered,this matched Volterra ROM greatly improves the accuracy of prediction.Moreover,the matched Volterra ROM,with the total number of step motions and thus the computational cost close to those of the conventional Volterra ROM method,has the additional advantage that the same set of kernels can match various translation motions with different starting conditions so the kernels can be predesigned without knowing the specific motion of airfoil.

关键词： Airfoil periodic translation Lift and drag Reduced-order model Transonic flow Unsteady flow

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Reverse metabolomics as a novel strategy to annotate the human metabolome

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Chinese Journal of Natural Medicines 2024年第4期22卷 289-290页

作者： YAN Tingting nie Liangliang HAO Haiping State Key Laboratory of Natural Medicines China Pharmaceutical UniversityNanjing 211198China Laboratory of Metabolic Regulation and Drug Target Discovery School of PharmacyChina Pharmaceutical UniversityNanjing 210009China

Identifying chemical structures inhuman-derived samples presents significant challenges due to limited structural data obtained from untargeted metabolomics studies.When the chemical structures of molecules are closely related to the phenotypic status of human ecosystems,it becomes invaluable to devise a method for efficiently and systematically determining structures that correlate with the pathophysiological status of humans in a high-throughput approach.

关键词： Reverse metabolomics Human metabolome Combinational synthesis Bile amidates

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Selective immobilization of Pb(Ⅱ)by biogenic whewellite and its mechanism

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Journal of Environmental Sciences 2024年第3期137卷 664-676页

作者： Xingxing Wang Kaiyan Ren Kairui Jiao Wenjun nie Xiaochi An Bin Lian College of Life Sciences College of Marine Science and EngineeringNanjing Normal UniversityNanjing 210023China

The development of bio-adsorbents with highly selective immobilization properties for specific heavy metals is a great challenge,but has important application value.Biogenic whewellite(BW)with high selectivity for Pb(Ⅱ)was synthesized by mineral microbial transformation.The selective immobilization properties and mechanism of BW for Pb(Ⅱ)were analyzed by combining mineral characterization technology and batch adsorption research methods.The results indicated that BW can efficiently and selectively immobilize Pb(Ⅱ)in single or composite heavy metal adsorption solutions,and the immobilized Pb(Ⅱ)is difficult to desorb.BW undergoes monolayer adsorption on Pb(Ⅱ),Qmax≈1073.17 mg/g.The immobilization of Pb(Ⅱ)by BW is a physico-chemical adsorption process with spontaneous heat absorption and an accompanying increase in entropy.In addition,the sequestration of Pb(Ⅱ)by BW remains around 756.99 mg/g even at p H=1.The excellent selective immobilization properties of BW for Pb(Ⅱ)are closely related to its smaller Ksp,electrostatic repulsion effect,organic-inorganic composite structure,acid resistance and the formation of Pb(Ⅱ)oxalate.This study provides beneficial information about the recycling of lead in acidic lead-containing wastewater and composite heavy metal contaminated water bodies.

关键词： Aspergillus niger Biogenic whewellite Pb(Ⅱ) Selective adsorption Immobilization mechanism

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Operational optimization of copper flotation process based on the weighted Gaussian process regression and index-oriented adaptive differential evolution algorithm

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Chinese Journal of Chemical Engineering 2024年第2期66卷 167-179页

作者： Zhiqiang Wang Dakuo He Haotian nie College of Information Science and Engineering Northeastern UniversityShenyang 110004China State Key Laboratory of Synthetical Automation for Process Industries Northeastern UniversityShenyang 110004China

Concentrate copper grade(CCG)is one of the important production indicators of copper flotation processes,and keeping the CCG at the set value is of great significance to the economic benefit of copper flotation industrial processes.This paper addresses the fluctuation problem of CCG through an operational optimization method.Firstly,a density-based affinity propagationalgorithm is proposed so that more ideal working condition categories can be obtained for the complex raw ore properties.Next,a Bayesian network(BN)is applied to explore the relationship between the operational variables and the CCG.Based on the analysis results of BN,a weighted Gaussian process regression model is constructed to predict the CCG that a higher prediction accuracy can be obtained.To ensure the predicted CCG is close to the set value with a smaller magnitude of the operation adjustments and a smaller uncertainty of the prediction results,an index-oriented adaptive differential evolution(IOADE)algorithm is proposed,and the convergence performance of IOADE is superior to the traditional differential evolution and adaptive differential evolution methods.Finally,the effectiveness and feasibility of the proposed methods are verified by the experiments on a copper flotation industrial process.

关键词： Weighted Gaussian process regression Index-oriented adaptive differential evolution Operational optimization Copper flotation process

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