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Insight into the selective separation of CO_(2)from biomass pyrolysis gas over metal-incorporated nitrogen-doped carbon materials:a first-principles study

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Frontiers of Chemical Science and Engineering 2024年第3期18卷 1-12页

作者： Li Zhao Xinru liu Zihao Ye bin Hu Haoyu wang Ji liu bing Zhang Qiang lu National Engineering Research Center of New Energy Power Generation North China Electric Power UniversityBeijing102206China

The composition of biomass pyrolysis gas is complex,and the selective separation of its components is crucial for its further utilization.Metal-incorporated nitrogen-doped materials exhibit enormous potential,whereas the relevant adsorption mechanism is still unclear.Herein,16 metal-incorporated nitrogen-doped carbon materials were designed based on the density functional theory calculation,and the adsorption mechanism of pyrolysis gas components H2,CO,CO_(2),CH_(4),and C2H6 was explored.The results indicate that metal-incorporated nitrogen-doped carbon materials generally have better adsorption effects on CO and CO_(2)than on H_(2),CH_(4),and C_(2)H_(6).Transition metal Mo-and alkaline earth metal Mg-and Ca-incorporated nitrogen-doped carbon materials show the potential to separate CO and CO_(2).The mixed adsorption results of CO_(2)and CO further indicate that when the CO_(2)ratio is significantly higher than that of CO,the saturated adsorption of CO_(2)will precede that of CO.Overall,the three metal-incorporated nitrogen-doped carbon materials can selectively separate CO_(2),and the alkaline earth metal Mg-incorporated nitrogen-doped carbon material has the best performance.This study provides theoretical guidance for the design of carbon capture materials and lays the foundation for the efficient utilization of biomass pyrolysis gas.

关键词： CO_(2)capture biomass pyrolysis gas selective adsorption carbon materials first-principles

Aggregation-induced T_(1)/T_(2) contrast enhancement for magnetic resonance imaging-guided intraoperative surgery

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Science China Chemistry 2024年第6期67卷 2046-2055页

作者： Wenbo Sun bin Yu Dianshuai Huang Chunhuan Jiang Wei wang Jianhua liu Zonghua wang Lehui lu State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun130022China College of Chemistry and Chemical Engineering Shandong Sino-Japanese Center for Collaborative Research of Carbon NanomaterialsQingdao Application Technology Innovation Center of Photoelectric Biosensing for Clinical Diagnosis and TreatmentQingdao UniversityQingdao266071China Department of Radiology Second Hospital of Jilin UniversityChangchun130041China

Magnetic resonance imaging(MRI)plays an important role in precision medicine that is hampered by the lack of contrast agents with high efficiency and the ability to translate diagnostic accuracy into therapeutic intervention.Herein,we demonstrate a DNA-based MRI probe that overcomes previous single-mode enhancement and provides a mechanism of action for aggregationinduced dual-modal MRI signal enhancement.A facile method is developed to produce aggregated T_(1)/T_(2)dual-modal NaGdF_(4):Dy@PDA-DNA(PDA=polydopamine)MRI probes.When aggregated,this probe can further amplify MRI signal intensity and exhibit improved geometrical and positional stability in vivo.The performance of the NaGdF_(4):Dy@PDA-DNA MRI probe toward MRI-guided preoperative planning and visualization-guided surgery is verified using an orthotopic tumor-bearing mouse model.The result shows that the rapid metabolism of the degraded probe leads to the mitigation of long-term toxic effects.Therefore,the developed high-performance MRI probe is of great significance for enhancing MRI diagnostic accuracy into precision medical therapeutic interventions.

关键词： MRI probe DNA aggregation-induced T_(1)/T_(2)contrast enhancement precision medicine degradable probe

维普期刊数据库

Regulating ion transport behaviors toward dendrite-free potassium metal batteries:recent advances and perspectives

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Rare Metals 2024年第4期43卷 1435-1460页

作者： lu-Kang Zhao Xuan-Wen Gao Tian-Zhen Ren Da wang Da-Wei wang Zhao-Meng liu Hong Chen Wen-bin luo School of Metallurgy Northeastern University School of Chemical Engineering The University of New South Wales

With abundant potassium resources and high capacity,potassium metal batteries（PMBs） present a compelling option for the next generation of energy storage technology.However,PMBs suffer from an unstable anode interface caused by uncontrolled dendrite growth,which results in unsatisfactory cyclability and safety concerns.Extensive investigations suggest that significant progress has been made in enhancing the interfacial stability of PMBs.The various effective strategies for stabilizing interfaces can ultimately be attributed to the regulation of the sluggish ion transfer kinetics and irregular deposition,i.e.,the arrangement of ion transport behaviors at the interface.Rational modulation of ions transport rate and ions deposition directions makes it possible to obtain a dendrite-free and smooth deposition plane.Herein,the influencing factors and action mechanism of K+interface transport behaviors are discussed to understand the nature of material design for constructing stable anode interfaces,including regulating the solvation and desolvation structures,accelerating K+transport kinetics and controlling K+deposition direction.In addition,the deficiencies and prospects of the research on electrolyte,separators and designed electrode involved in the manufacturing and testing and ion transport process of PMBs are discussed.This review is expected to provide some possible directions for constructing dendrite-free interfaces in advanced PMBs-related research and offer significant insights for prospective experimental research and commercial applications.

关键词： Ion transport rate Ion transport direction Interface Potassium metal batteries Dendrites growth

Synthesis-temperature-dependent phase composition manipulation toward high thermoelectric performance in tetrahedrites

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Journal of Materials Science & Technology 2024年第1期168卷 124-130页

作者： Yiqing Wei Jiaqi liu Zien Cheng Pengfei Jiang Zizhen Zhou bin Zhang Guoyu wang Guang Han Xu lu Xiaoyuan Zhou Center of Quantum Materials and Devices College of PhysicsChongqing UniversityChongqing 401331China College of Materials Science and Engineering Chongqing UniversityChongqing 400044China College of Chemistry and Chemical Engineering Chongqing UniversityChongqing 401331China Analytical and Testing Center Chongqing UniversityChongqing 401331China

Tetrahedrite,an Earth-abundant natural mineral,has attracted extensive research interest because of its excellent thermoelectric performance.Herein,tetrahedrite samples comprising Cu-poor Cu_(12)Sb_(4)S_(13)and Cu-rich Cu_(14)Sb_(4)S_(13)phases have been synthesized using a colloidal method,in which the ratio of two phases is manipulated by controlling the synthesis temperature to improve the thermoelectric perfor-mance.It is found that an ultralow total thermal conductivity of∼0.3 W m^(−1)K^(−1)at 723 K is realized in the sample with a Cu-rich phase fraction of∼50%,which can be attributed to maximized phonon scattering by phase boundaries.As a result,combined with a decent power factor,this sample obtains an optimal zT of 1.15,which is about 85%higher than that of the sample with a Cu-rich phase fraction of∼64%and comparable to zT values of other eco-friendly,abundant Cu-based thermoelectric materials.This work demonstrates an effective synthesis-temperature-dependent phase composition manipulation strategy toward enhanced thermoelectric performance in tetrahedrites.

关键词： Tetrahedrite Thermoelectric Colloidal method Phase manipulation Thermal conductivity

Mechanical robust and self-healing flexible perovskite solar cells with efficiency exceeding 23%

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Science China Chemistry 2024年第8期67卷 2670-2678页

作者： Yaohua wang Ruikun Cao Yuanyuan Meng bin Han Ruijia Tian Xiaoyi lu Zhenhua Song Shuncheng Yang Congda lu Chang liu Ziyi Ge College of Mechanical Engineering Zhejiang University of Technology Zhejiang Provincial Engineering Research Center of Energy Optoelectronic Materials and Devices Ningbo Institute of Materials Technology& Engineering Chinese Academy of Sciences Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences

Flexible perovskite solar cells(f-PSCs) have experienced rapid advancements due to the light-weight, flexibility, and solution processability of the perovskite materials, which prompted the power conversion efficiency(PCE) to 24.08%. However, f-PSCs still face challenges in terms of mechanical and environmental stability. This is primarily due to their inherent brittleness, the presence of residual tensile strain, and the high density of defects along the boundaries of perovskite grains. To this end, we carefully developed a cross-linkable elastomers 3-[(3-acrylamidopropyl)dimethylammonium] propanoate(ADP) with electrostatic dynamic bond, which could be in-situ cross-linked and coordinate with [Pb I6]4-to regulate the crystallization process of perovskite. The cross-linked elastomers attached to the perovskite grain boundaries could release the remaining tensile strains and mechanical stresses, leading to enhanced stability and flexibility of the f-PSCs. More importantly, the electrostatic interaction between positive and negative groups of cross-linked elastomers and hydrogen bond formation between N–H and C=O accelerate the cross-linking of ADP, endowing the flexible perovskite films with self-healing ability under mild treating conditions(60 °C for 30 min). As a result, the device achieves a remarkable PCE of 23.53%(certified 23.16%). Additionally, the device exhibits impressive mechanical sustainability and durability, retaining over 90% of initial PCE even after undergoing8,000 bending cycles.

关键词： PERFORMANCE STABILITY

Phase field modeling of grain stability of nanocrystalline alloys by explicitly incorporating mismatch strain

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Rare Metals 2024年第7期43卷 3370-3382页

作者： Min Zhou Hong-Hui Wu Yuan Wu Hui wang Xiong-Jun liu Sui-He Jiang Xiao-bin Zhang Zhao-Ping lu Beijing Advanced Innovation Center for Materials Genome Engineering State Key Laboratory for Advanced Metals and MaterialsUniversity of Science and Technology Beijing Institute for Carbon Neutrality University of Science and Technology Institute of Materials Intelligent Technology Liaoning Academy of Materials

Ab st ra ct Nanocrystalline materials exhibit unique properties due to their extremely high grain boundary(GB) density.However,this high-density characteristic induces grain coarsening at elevated temperatures,thereby limiting the widespread application of nanocrystalline materials.Recent experimental observations revealed that GB segregation and second-phase pinning effectively hinder GB migration,thereby improving the stability of nanocry stalline materials.In this study,a mouified phase-field model that integrates mismatch strain,solute segregation and precipitation was developed to evaluate the influence of lattice misfit on the thermal stability of nanocrystalline alloys.The simulation results indicated that introducing a suitable mismatch strain can effectively enhance the microstructural stability of nanocrystalline alloys.By synergizing precipitation with an appropriate lattice misfit,the formation of second-phase particles in the bulk grains can be suppressed,thereby facilitating solute segregation/precipitation at the GBs.This concentrated solute segregation and precipitation at the GBs effectively hinders grain migration,thereby preventing grain coarsening.These findings provide a new perspective on the design and regulation of nanocrystalline alloys with enhanced thermal stability.

关键词： Phase field model Mismatch strain Second-phase precipitation Grain boundary segregation Nanocrystalline alloys

Controlled Synthesis of Proton-Conductive Porous Organic Polymer Gels via Electrostatically Stabilized Colloidal Formation

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CCS Chemistry 2024年第7期6卷 1767-1775页

作者： bin Chen Yifeng Kuang lu liu Linkun Cai Zaoming wang Panchao Yin Liangbin Huang Cheng Gu State Key Laboratory of luminescent Materials and Devices Institute of Polymer Optoelectronic Materials and DevicesSouth China University of TechnologyGuangzhou 510640 College of Polymer Science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065 Key Laboratory of Functional Molecular Engineering of Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510641 South China Advanced Institute for Soft Matter Science and Technology South China University of TechnologyGuangzhou 510640 Institute for Integrated Cell-Material Sciences Institute for Advanced StudyKyoto UniversityKyoto 606-8501

Porous organic polymers(POPs)have attracted extensive interest due to their structural diversity and predesigned functionality.However,the majority of POPs are synthesized as insoluble and unprocessable powders,which greatly impede their advanced applications because of limited mass transport and inadaptation for device integration.Herein,we report a controlled synthetic strategy of macroscopic POP gels by a cation-stabilized colloidal formation mechanism,which is widely adaptable to a large variety of tetra-/tri-amino build blocks for the synthesis of Tröger’s base-linked POP gels,aerogels,and ionic gels.The POP gels combined the integrated advantages of hierarchically porous structures and tailorable mechanical stiffness,whereas they could load substantial amounts of phosphoric acids and construct unimpeded transport pathways for proton conduction,exhibiting unprecedented proton conductivity at subzero temperatures.Our strategy offers a new solution to the intractable processing issues of POPs toward device applications with cutting-edge performances.

关键词： porous organic polymers Tröger’s base linkage gels superprotonic conduction subzero temperatures

Integrating machine learning and CALPHAD method for exploring low-modulus near-β-Ti alloys

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Rare Metals 2024年第1期43卷 309-323页

作者： Hao Zou Yue-Yan Tian Li-Gang Zhang Ren-Hao Xue Zi-Xuan Deng Ming-Ming lu Jian-Xin wang Li-bin liu School of Computer Science and Engineering Central South UniversityChangsha 410083China School of Materials Science and Engineering Central South UniversityChangsha 410083China State Key Laboratory of Powder Metallurgy Central South UniversityChangsha 410083China

Traditional theoretical and empirical calculation methods can guide the design of β-and metastable β-alloys for bio-titanium. However, it is still difficult to obtain novel near-β-Ti alloys with low modulus. This study developed a method that combines machine learning with calculation of phase diagrams(CALPHAD) to facilitate the design of near-β-Ti alloys. An elastic modulus database of Ti–Nb–Zr–Mo–Ta–Sn system was constructed first, and then three features(the electron to atom ratio, mean absolute deviation of atom mass, and mean electronegativity) were selected as the key factors of modulus by performing a three-step feature selection. With these features, a highly accurate model was built for predicting the modulus of near-β-Ti alloys. To further ensure the accuracy of modulus prediction, machine learning with the elastic constants calculated was leveraged by CALPHAD database. The root mean square error of the well-trained model can be as low as 6.75 GPa. Guided by the prediction of machine learning and CALPHAD, three novel near-β-Ti alloys with elastic modulus below 50 GPa were successfully designed in this study. The best candidate alloy(Ti–26Nb–4Zr–4Sn–1Mo–Ta) exhibits an ultra-low modulus(36.6 GPa) after cold rolling with a thickness reduction of 20%. Our method can greatly save time and resources in the development of novel Ti alloys, and experimental verifications have demonstrated the reliability of this method.

关键词： Near-β-Ti alloy Machine learning Calculation of phase diagram Low-modulus alloy Feature selection

维普期刊数据库

Unveiling size-fluorescence correlation of organic nanoparticles and its use in nanoparticle size determination

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Aggregate 2024年第1期5卷 331-336页

作者： Wu-Jie Guo Shixiang Ma Hui wang lu Qiao Lei Chen Chenyu Hong bin liu Xiaoyan Zheng Hui-Qing Peng State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and EngineeringBeijing University of Chemical TechnologyBeijingChina Key Laboratory of Cluster Science of Ministry of Education Beijing Key Laboratory of Photoelectronic/Electro-photonic Conversion MaterialsKey Laboratory of Medicinal Molecule Science and Pharmaceutics Engineering of Ministry of Industry and Information TechnologySchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijingChina

Quantitatively establishing the correlation between nanoparticle size and fluorescence is essential for understanding the behavior and functionality of fluorescent nanoparticles(FNPs).However,such exploration focusing on organic FNPs has not been achieved to date.Herein,we employ the use of supramolecular polymeric FNPs prepared from tetraphenylethylene-based bis-ureidopyrimidinone monomers(bis-UPys)to relate the size to the fluorescence of organic nanoparticles.At an equal concentration of bis-UPys,a logarithmic relationship between them is built with a correlation coefficient higher than 0.96.Theoretical calculations indicate that variations in fluorescence intensity among FNPs of different sizes are attributed to the distinct molecular packing environments at the surface and within the interior of the nanoparticles.This leads to different nonradiative decay rates of the embedded and exposed bis-UPys and thereby changes the overall fluorescence quantum yield of nanoparticles due to their different specific surface areas.The established fluorescence intensity-size correlation possesses fine universality and reliability,and it is successfully utilized to estimate the sizes of other nanoparticles,including those in highly diluted dispersions of FNPs.This work paves a new way for the simple and real-time determination of nanoparticle sizes and offers an attractive paradigm to optimize nanoparticle functionalities by the size effect.

关键词： aggregation-induced emission fluorescence detection fluorescent nanoparticle nanoparticle size supramolecular polymer