Micro/nanorobots can propel and navigate in many hard-to-reach biological environments,and thus may bring revolutionary changes to biomedical research and applications.However,current MNRs lack the capability to colle...Micro/nanorobots can propel and navigate in many hard-to-reach biological environments,and thus may bring revolutionary changes to biomedical research and applications.However,current MNRs lack the capability to collectively perceive and report physicochemical changes in unknown microenvironments.Here we propose to develop swarming responsive photonic nanorobots that can map local physicochemical conditions on the fly and further guide localized photothermal treatment.The RPNRs consist of a photonic nanochain of periodically-assembled magnetic Fe_(3)O_(4)nanoparticles encapsulated in a responsive hydrogel shell,and show multiple integrated functions,including energetic magnetically-driven swarming motions,bright stimuli-responsive structural colors,and photothermal conversion.Thus,they can actively navigate in complex environments utilizing their controllable swarming motions,then visualize unknown targets(e.g.,tumor lesion)by collectively mapping out local abnormal physicochemical conditions(e.g.,pH,temperature,or glucose concentra-tion)via their responsive structural colors,and further guide external light irradiation to initiate localized photothermal treatment.This work facilitates the development of intelligent motile nanosensors and versatile multifunctional nanotheranostics for cancer and inflam-matory diseases.展开更多
Cadmium selenide(CdSe)is an inorganic semiconductor with unique optical and electronic properties that make it useful in various applications,including solar cells,light-emitting diodes,and biofluorescent tagging.In o...Cadmium selenide(CdSe)is an inorganic semiconductor with unique optical and electronic properties that make it useful in various applications,including solar cells,light-emitting diodes,and biofluorescent tagging.In order to synthesize high-quality crystals and subsequently integrate them into devices,it is crucial to understand the atomic scale crystallization mechanism of CdSe.Unfortunately,such studies are still absent in the literature.To overcome this limitation,we employed an enhanced sampling-accelerated active learning approach to construct a deep neural potential with ab initio accuracy for studying the crystallization of CdSe.Our brute-force molecular dynamics simulations revealed that a spherical-like nu-cleus formed spontaneously and stochastically,resulting in a stacking disordered structure where the competition between hexagonal wurtzite and cubic zinc blende polymorphs is temperature-dependent.We found that pure hexagonal crystal can only be obtained approximately above 1430 K,which is 35 K below its melting temperature.Furthermore,we observed that the solidification dynamics of Cd and Se atoms were distinct due to their different diffusion coefficients.The solidification process was initiated by lower mobile Se atoms forming tetrahedral frameworks,followed by Cd atoms occupying these tetra-hedral centers and settling down until the third-shell neighbor of Se atoms sited on their lattice posi-tions.Therefore,the medium-range ordering of Se atoms governs the crystallization process of CdSe.Our findings indicate that understanding the complex dynamical process is the key to comprehending the crystallization mechanism of compounds like CdSe,and can shed lights in the synthesis of high-quality crystals.展开更多
The rational design of platinum-based electrocatalysts with optimized metal-support electronic interactions remains a fundamental challenge in achieving atom-efficient hydrogen evolution reaction(HER).This study demon...The rational design of platinum-based electrocatalysts with optimized metal-support electronic interactions remains a fundamental challenge in achieving atom-efficient hydrogen evolution reaction(HER).This study demonstrates a coordination-driven synthesis strategy to engineer highly dispersed ultra-smallα-MoC_(1-x)anchored on nitrogen-doped carbon(NC)frameworks,leveraging the unique metal-organic coordination chemistry between molybdenum species and imidazolate ligands in ZIF-8 precursors.Through precise control of the carbide crystallization process,we establish an atomic-level interface configuration that enables the preferential anchoring of Pt atoms onto the metastableα-MoC_(1-x)phase.The resulting strong metal-support interaction(SMSI)induces significant electron redistribution at the Pt/α-MoC_(1-x)interface,as evidenced by X-ray absorption spectroscopy(XAS).The optimized Pt/α-MoC_(1-x)/NC architecture demonstrates exceptional HER performance with low overpotentials of 19 and 84 mV at current density of 10 and 100 mA·cm^(-2).Remarkably,it achieves a mass activity of 15.3 A·mgPt^(-1)at 100 mV overpotential,10.9-fold enhancement compared to commercial 20%Pt/C(1.4 A·mgPt^(-1)).This work establishes a new paradigm for constructing interfacial electronic environments through support dispersion engineering,providing fundamental insights into the design principles of high-efficiency catalysts for sustainable hydrogen production.展开更多
The rapid advancements in artificial intelligence(AI)are catalyzing transformative changes in atomic modeling,simulation,and design.AI-driven potential energy models havedemonstrated the capability to conduct large-sc...The rapid advancements in artificial intelligence(AI)are catalyzing transformative changes in atomic modeling,simulation,and design.AI-driven potential energy models havedemonstrated the capability to conduct large-scale,long-duration simulations with the accuracy of ab initio electronic structure methods.However,the model generation process remains a bottleneck for large-scale applications.We propose a shift towards a model-centric ecosystem,wherein a large atomic model(LAM),pretrained across multiple disciplines,can be efficiently fine-tuned and distilled for various downstream tasks,thereby establishing a new framework for molecular modeling.In this study,we introduce the DPA-2 architecture as a prototype for LAMs.Pre-trained on a diverse array of chemical and materials systemsusing a multi-task approach,DPA-2demonstrates superior generalization capabilities across multiple downstream tasks compared to the traditional single-task pre-training and fine-tuning methodologies.Our approach sets the stage for the development and broad application of LAMs in molecular and materials simulation research.展开更多
Swarming magnetic micro/nanorobots hold great promise for biomedical applications,but at present suffer from inferior capabilities to perceive and respond to chemical signals in local microenvironments.Here we demonst...Swarming magnetic micro/nanorobots hold great promise for biomedical applications,but at present suffer from inferior capabilities to perceive and respond to chemical signals in local microenvironments.Here we demonstrate swarming magnetic photonic crystal microrobots(PC-bots)capable of sponta-neously performing on-the-fly visual pH detection and self regulated drug delivery by perceiving local pH changes.The magnetic PC-bots consist of pH-responsive hydrogel microspheres with encapsulated one-dimensional periodic assemblies of Fe3O4 nanoparticles.By programming extemnal rotating magnetic fields,they can self-organize into large swarms with much-enhanced collective velocity to actively find targets while shining bright“blinking”structural colors.When approaching the target with abnormal pH conditions(e.g.an ulcerated superficial tumor lesion),the PC-bots can visualize local pH changes on the fly via pH-responsive structural colors,and realize self-regulated release of the loaded drugs by recognizing local pH.This work facilita tes the develop-ment of intelligent micro/nanorobots for active“motile-targeting”tumor diag-nosis and treatment.展开更多
基金supported by the National Key Research and Development Project(No.2021YFA1201400)National Natural Science Foundation of China(Nos.52073222,51573144 and 21474078)the Fundamental Research Funds for the Central Universities(WUT:2021IVA118 and 2022IVA201).
文摘Micro/nanorobots can propel and navigate in many hard-to-reach biological environments,and thus may bring revolutionary changes to biomedical research and applications.However,current MNRs lack the capability to collectively perceive and report physicochemical changes in unknown microenvironments.Here we propose to develop swarming responsive photonic nanorobots that can map local physicochemical conditions on the fly and further guide localized photothermal treatment.The RPNRs consist of a photonic nanochain of periodically-assembled magnetic Fe_(3)O_(4)nanoparticles encapsulated in a responsive hydrogel shell,and show multiple integrated functions,including energetic magnetically-driven swarming motions,bright stimuli-responsive structural colors,and photothermal conversion.Thus,they can actively navigate in complex environments utilizing their controllable swarming motions,then visualize unknown targets(e.g.,tumor lesion)by collectively mapping out local abnormal physicochemical conditions(e.g.,pH,temperature,or glucose concentra-tion)via their responsive structural colors,and further guide external light irradiation to initiate localized photothermal treatment.This work facilitates the development of intelligent motile nanosensors and versatile multifunctional nanotheranostics for cancer and inflam-matory diseases.
基金supported by the National Natural Science Foundation of China(No.92370118)the National Science Fund for Excellent Young Scientist Fund Program(Overseas)of China,the Science and Technology Activities Fund for Overseas Researchers of Shaanxi Province,China,and the Research Fund of the State Key Laboratory of Solidification Proceeding(NPU)of China(No.2020-QZ-03).
文摘Cadmium selenide(CdSe)is an inorganic semiconductor with unique optical and electronic properties that make it useful in various applications,including solar cells,light-emitting diodes,and biofluorescent tagging.In order to synthesize high-quality crystals and subsequently integrate them into devices,it is crucial to understand the atomic scale crystallization mechanism of CdSe.Unfortunately,such studies are still absent in the literature.To overcome this limitation,we employed an enhanced sampling-accelerated active learning approach to construct a deep neural potential with ab initio accuracy for studying the crystallization of CdSe.Our brute-force molecular dynamics simulations revealed that a spherical-like nu-cleus formed spontaneously and stochastically,resulting in a stacking disordered structure where the competition between hexagonal wurtzite and cubic zinc blende polymorphs is temperature-dependent.We found that pure hexagonal crystal can only be obtained approximately above 1430 K,which is 35 K below its melting temperature.Furthermore,we observed that the solidification dynamics of Cd and Se atoms were distinct due to their different diffusion coefficients.The solidification process was initiated by lower mobile Se atoms forming tetrahedral frameworks,followed by Cd atoms occupying these tetra-hedral centers and settling down until the third-shell neighbor of Se atoms sited on their lattice posi-tions.Therefore,the medium-range ordering of Se atoms governs the crystallization process of CdSe.Our findings indicate that understanding the complex dynamical process is the key to comprehending the crystallization mechanism of compounds like CdSe,and can shed lights in the synthesis of high-quality crystals.
基金supported by the National Key R&D Program of China(No.2021YFA1501102)the National Natural Science Foundation of China(Nos.22276023,22472019,22409133,22172083)+1 种基金the Fundamental Research Funds for the Central Universities(No.DUT22LAB602)Liaoning Binhai Laboratory Project(No.LBLF-202306).
文摘The rational design of platinum-based electrocatalysts with optimized metal-support electronic interactions remains a fundamental challenge in achieving atom-efficient hydrogen evolution reaction(HER).This study demonstrates a coordination-driven synthesis strategy to engineer highly dispersed ultra-smallα-MoC_(1-x)anchored on nitrogen-doped carbon(NC)frameworks,leveraging the unique metal-organic coordination chemistry between molybdenum species and imidazolate ligands in ZIF-8 precursors.Through precise control of the carbide crystallization process,we establish an atomic-level interface configuration that enables the preferential anchoring of Pt atoms onto the metastableα-MoC_(1-x)phase.The resulting strong metal-support interaction(SMSI)induces significant electron redistribution at the Pt/α-MoC_(1-x)interface,as evidenced by X-ray absorption spectroscopy(XAS).The optimized Pt/α-MoC_(1-x)/NC architecture demonstrates exceptional HER performance with low overpotentials of 19 and 84 mV at current density of 10 and 100 mA·cm^(-2).Remarkably,it achieves a mass activity of 15.3 A·mgPt^(-1)at 100 mV overpotential,10.9-fold enhancement compared to commercial 20%Pt/C(1.4 A·mgPt^(-1)).This work establishes a new paradigm for constructing interfacial electronic environments through support dispersion engineering,providing fundamental insights into the design principles of high-efficiency catalysts for sustainable hydrogen production.
基金supported by the National Key R&D Program of China(grantno.2022YFA1004300)the National Natural Science Foundation of China(grant no.12122103)+11 种基金supported by the National Key Research and Development Project of China(grant no.2022YFA1004302)the National Natural Science Foundation of China(grants nos.92270001 and 12288101)supported by the National Institutes of Health(grant no.GM107485 to D.M.Y.)the National Science Foundation(grant no.2209718 to D.M.Y.)supported by the Natural Science Foundation of Zhejiang Province(grant no.2022XHSJJ006)supported by the National Natural Science Foundation of China(grants nos.22222303 and 22173032)supported by the National Key R&D Program of China(grants nos.2021YFA0718900 and 2022YFA1403000)supported by the National Natural Science Foundation of China(grants nos.12034009 and 91961204)supported by the National Science Fund for Distinguished Young Scholars(grant no.22225302)Laboratory of AI for Electrochemistry(AI4EC),and IKKEM(grants nos.RD2023100101 and RD2022070501)supported by the National Natural Science Foundation of China(grants nos.12122401,12074007,and 12135002)Lastly,the computational resource was supported by the Bohrium Cloud Platform at DP Technology and Tan Kah Kee Supercomputing Center(IKKEM).
文摘The rapid advancements in artificial intelligence(AI)are catalyzing transformative changes in atomic modeling,simulation,and design.AI-driven potential energy models havedemonstrated the capability to conduct large-scale,long-duration simulations with the accuracy of ab initio electronic structure methods.However,the model generation process remains a bottleneck for large-scale applications.We propose a shift towards a model-centric ecosystem,wherein a large atomic model(LAM),pretrained across multiple disciplines,can be efficiently fine-tuned and distilled for various downstream tasks,thereby establishing a new framework for molecular modeling.In this study,we introduce the DPA-2 architecture as a prototype for LAMs.Pre-trained on a diverse array of chemical and materials systemsusing a multi-task approach,DPA-2demonstrates superior generalization capabilities across multiple downstream tasks compared to the traditional single-task pre-training and fine-tuning methodologies.Our approach sets the stage for the development and broad application of LAMs in molecular and materials simulation research.
基金National Key Research and Development Program,Grant/Award Numbers:2021YFA1201400,2022YF B4701700National Natural Science Foundation of China,Grant/Award Numbers:21875175,52073222,52175009+3 种基金Interdisciplinary Research Foundation of HIT,Grant/Award Number:1R20211219Natural Science Foundation of Chonging,Grant/Award Number:CSTB2022NSCQ-MSX0507Natural Science Foundation of Heilongian Province,Grant/Award Number.YQ2022E022Central University Basic Research Fund of China,Grant/Award Number:2022IVA201。
文摘Swarming magnetic micro/nanorobots hold great promise for biomedical applications,but at present suffer from inferior capabilities to perceive and respond to chemical signals in local microenvironments.Here we demonstrate swarming magnetic photonic crystal microrobots(PC-bots)capable of sponta-neously performing on-the-fly visual pH detection and self regulated drug delivery by perceiving local pH changes.The magnetic PC-bots consist of pH-responsive hydrogel microspheres with encapsulated one-dimensional periodic assemblies of Fe3O4 nanoparticles.By programming extemnal rotating magnetic fields,they can self-organize into large swarms with much-enhanced collective velocity to actively find targets while shining bright“blinking”structural colors.When approaching the target with abnormal pH conditions(e.g.an ulcerated superficial tumor lesion),the PC-bots can visualize local pH changes on the fly via pH-responsive structural colors,and realize self-regulated release of the loaded drugs by recognizing local pH.This work facilita tes the develop-ment of intelligent micro/nanorobots for active“motile-targeting”tumor diag-nosis and treatment.
