Nitrate synthesis is an important process for agriculture and industry,but suffers from energy-intensive steps including the synthesis and subsequent oxidation of ammonia.Herein,we present a selective N_(2)transformat...Nitrate synthesis is an important process for agriculture and industry,but suffers from energy-intensive steps including the synthesis and subsequent oxidation of ammonia.Herein,we present a selective N_(2)transformation to nitrate by guiding the charge neutralization of self-electrified water microdroplets in an artificial cloud generated with the portable ultrasonic atomizer.The electron and ion transfer in the charge neutralization of water microdroplets on metal micromesh enables an up to~40-fold increase in the reactivity of nitrate formation reaction driven by ultrasonic energy.A robust semi-continuous N_(2)oxidation by a Ni-mesh-screened cloud system was achieved,providing nitrate with~12 mM concentration every 20 h.These findings emphasize the potential of harnessing the microdroplet-mediated cloud electrochemistry of N_(2)in decentralizing the current mass production of fertilizer.展开更多
Droplet impact on solid surfaces plays a critical role in a wide range of applications,including inkjet printing,spray cooling,surface coatings,and microdroplet chemistry.Precise control of droplet–surface interactio...Droplet impact on solid surfaces plays a critical role in a wide range of applications,including inkjet printing,spray cooling,surface coatings,and microdroplet chemistry.Precise control of droplet–surface interactions is essential,but the fundamental mechanisms governing this process are still not fully understood.In this study,we demonstrate that large contact angle hysteresis(CAH)on hydrophobic nanoporous surfaces significantly amplifies post-impact droplet oscillations.This reveals the critical influence of CAH on the redistribution of impact energy and the modulation of droplet–surface interactions.Using shape mode decomposition via Legendre polynomials and fast Fourier transform spectral analysis,we show that surfaces with larger CAH excite and sustain higher-order droplet shape mode oscillations,leading to persistent capillary waves even after contact line pinning.The observed amplitude modulation and multiple frequency components within individual shape modes reveal nonlinear energy transfer between different modes.These amplified and coupled oscillations are shown to promote daughter droplet coalescence.This study presents a framework for understanding the role of CAH in storing and redistributing impact energy through nonlinear mode excitation and establishes CAH as a critical design parameter for controlling fluid dynamics on solid surfaces.展开更多
Biopolymers, including DNA and peptides have been used as excellent self-assembling building blocks for programmable single-component or hybrid materials, due to their controlled molecular interactions.However, combin...Biopolymers, including DNA and peptides have been used as excellent self-assembling building blocks for programmable single-component or hybrid materials, due to their controlled molecular interactions.However, combining two assembling principles of DNA-based programmability and peptide-based specific molecular interactions for hybrid structures to microscale has not yet been achieved. In this study,we describe a hybrid microsystem that emerges from the co-assembly of DNA origami structure and short elastin-like polypeptide conjugated oligonucleotides, and initiates liquid-liquid phase separation to generate microdroplets upon heating above the transition temperature. Moreover, the hybrid microdroplets are capable for vip molecule trapping and perform bi-/tri-enzymatic cascades with rate enhancements as open “microreactors”. Our programmed assembled DNA-peptide microsystem represents a new combination of DNA nanotechnology and peptide science and opens potential application routes toward lifeinspired biomaterials.展开更多
Study of stable liquid crystal(LC)microdroplets is of great significance for LC dynamics in con fined space or at topological surface.However,the fabrication of LC microdroplets with diverse shape without ionic gelati...Study of stable liquid crystal(LC)microdroplets is of great significance for LC dynamics in con fined space or at topological surface.However,the fabrication of LC microdroplets with diverse shape without ionic gelati on agents still remai ns challe nging due to the fluid instability.Here,we utilize the microfluidic tech no logy to prepare graphe ne oxide(GO)LC microdroplets with various morphologies based on the anomalous rheological property of GO aqueous dispersion.Different from LC of one-dimensional polymer,LC containing two-dimensional GO sheets exhibits considerable viscoelasticity and weak extensibility,resulting from the planar molecular conformation and the absence of intermolecular entangleme nts.The low exte risibility ensures that GO aqueous suspension is discretized into mono dispersed microdroplets rather than thin thread in the microfluidic channels.The large viscoelasticity and ultra-1 ong relaxation time of GO LC enable the diverse stable morphologies of microdroplets.The droplet morphology is well con trolled from sphere to teardrop by modulati ng the competition between GO viscoelasticity and in terfacial ten sion.The two-dimensional GO LC featuri ng unique rheological property provides a novel system for the microfluidic field,and corresponding topological stability enriches the LC dyn amics and ope ns a new pathway for desig ning graphe ne-based materials.展开更多
ABSTRACT The Raman intensitics of gas molecules were found to be enormously enhanced in the presence of Hg-microdroplets.The enhancement factor for the molecules studied was found to be over 20.
The crystallization of ionic crystals has traditionally been explained by Gibbs's classical nucleation theory.However,recent observations of intermediate phases during nucleation suggest that the process may be mo...The crystallization of ionic crystals has traditionally been explained by Gibbs's classical nucleation theory.However,recent observations of intermediate phases during nucleation suggest that the process may be more complex,necessitating new theoretical frameworks,though key empirical evidence remains elusive.In this study,we used microdroplets to investigate the crystallization of sodium halides(NaCl,NaBr,and NaI)under homogeneous nucleation conditions across a wide range of supersaturations.In the evaporating droplet,NaCl follows the classical nucleation pathway,whereas NaBr and NaI exhibit the formation of an intermediate phase prior to the nucleation of anhydrous and hydrous single crystals,respectively.Optical and computational analyses indicate that these intermediate phases are liquid crystal phases composed of contact ion pairs.These findings establish a new theoretical framework for crystal nucleation and growth and offer methods to control nucleation pathways,enabling us to achieve desired crystals regardless of specific conditions.展开更多
基金supported by the National Key R&D Program of China(2022YFA1504603)the National Natural Science Foundation of China(22025206,22172163)+1 种基金the Dalian Innovation Support Plan for High Level Talents(2022RG13)the Fundamental Research Funds for the Central Universities(20720220008)。
文摘Nitrate synthesis is an important process for agriculture and industry,but suffers from energy-intensive steps including the synthesis and subsequent oxidation of ammonia.Herein,we present a selective N_(2)transformation to nitrate by guiding the charge neutralization of self-electrified water microdroplets in an artificial cloud generated with the portable ultrasonic atomizer.The electron and ion transfer in the charge neutralization of water microdroplets on metal micromesh enables an up to~40-fold increase in the reactivity of nitrate formation reaction driven by ultrasonic energy.A robust semi-continuous N_(2)oxidation by a Ni-mesh-screened cloud system was achieved,providing nitrate with~12 mM concentration every 20 h.These findings emphasize the potential of harnessing the microdroplet-mediated cloud electrochemistry of N_(2)in decentralizing the current mass production of fertilizer.
基金supported by the German Federal Ministry of Education and Research(BMBF)within the project H2Giga-SINEWAVE OxySep,grant no 03HY123Eand the Faculty of Mechanical Science and Engineering at TU Dresden.Pengfei Zhao would like to acknowledge the China Scholarship Council(CSC)+3 种基金supported by a Humboldt Research Fellowship from the Alexander von Humboldt Foundationthe financial support from Qinghai Province(No.2025ZY001,2024000060)Chinese Academy of Sciences(No.2023000024)funding from the Deutsche Forschungsgemeinschaft:Project ID 265191195-SFB1194 and 456180046.
文摘Droplet impact on solid surfaces plays a critical role in a wide range of applications,including inkjet printing,spray cooling,surface coatings,and microdroplet chemistry.Precise control of droplet–surface interactions is essential,but the fundamental mechanisms governing this process are still not fully understood.In this study,we demonstrate that large contact angle hysteresis(CAH)on hydrophobic nanoporous surfaces significantly amplifies post-impact droplet oscillations.This reveals the critical influence of CAH on the redistribution of impact energy and the modulation of droplet–surface interactions.Using shape mode decomposition via Legendre polynomials and fast Fourier transform spectral analysis,we show that surfaces with larger CAH excite and sustain higher-order droplet shape mode oscillations,leading to persistent capillary waves even after contact line pinning.The observed amplitude modulation and multiple frequency components within individual shape modes reveal nonlinear energy transfer between different modes.These amplified and coupled oscillations are shown to promote daughter droplet coalescence.This study presents a framework for understanding the role of CAH in storing and redistributing impact energy through nonlinear mode excitation and establishes CAH as a critical design parameter for controlling fluid dynamics on solid surfaces.
基金supported by the National Natural Science Foundation of China (No. 31600802)。
文摘Biopolymers, including DNA and peptides have been used as excellent self-assembling building blocks for programmable single-component or hybrid materials, due to their controlled molecular interactions.However, combining two assembling principles of DNA-based programmability and peptide-based specific molecular interactions for hybrid structures to microscale has not yet been achieved. In this study,we describe a hybrid microsystem that emerges from the co-assembly of DNA origami structure and short elastin-like polypeptide conjugated oligonucleotides, and initiates liquid-liquid phase separation to generate microdroplets upon heating above the transition temperature. Moreover, the hybrid microdroplets are capable for vip molecule trapping and perform bi-/tri-enzymatic cascades with rate enhancements as open “microreactors”. Our programmed assembled DNA-peptide microsystem represents a new combination of DNA nanotechnology and peptide science and opens potential application routes toward lifeinspired biomaterials.
基金by the National Natural Science Foundation of China(Nos.52090030,51533008,51703194,51973191,51873191 and 51803177)National Key R&D Program of China(No.2016YFA0200200),Hundred Talents Program of Zhejiang University(No.188020*194231701/113),Key Research and Development Plan of Zhejiang Province(2018C01049)+1 种基金the Fundamental Research Funds for the Central Universities(No.K20200060)Key Laboratory of Novel Adsorpti on and Separati on Materials and Applicatio n Technology of Zhejiang Province(No.512301-121502).
文摘Study of stable liquid crystal(LC)microdroplets is of great significance for LC dynamics in con fined space or at topological surface.However,the fabrication of LC microdroplets with diverse shape without ionic gelati on agents still remai ns challe nging due to the fluid instability.Here,we utilize the microfluidic tech no logy to prepare graphe ne oxide(GO)LC microdroplets with various morphologies based on the anomalous rheological property of GO aqueous dispersion.Different from LC of one-dimensional polymer,LC containing two-dimensional GO sheets exhibits considerable viscoelasticity and weak extensibility,resulting from the planar molecular conformation and the absence of intermolecular entangleme nts.The low exte risibility ensures that GO aqueous suspension is discretized into mono dispersed microdroplets rather than thin thread in the microfluidic channels.The large viscoelasticity and ultra-1 ong relaxation time of GO LC enable the diverse stable morphologies of microdroplets.The droplet morphology is well con trolled from sphere to teardrop by modulati ng the competition between GO viscoelasticity and in terfacial ten sion.The two-dimensional GO LC featuri ng unique rheological property provides a novel system for the microfluidic field,and corresponding topological stability enriches the LC dyn amics and ope ns a new pathway for desig ning graphe ne-based materials.
文摘ABSTRACT The Raman intensitics of gas molecules were found to be enormously enhanced in the presence of Hg-microdroplets.The enhancement factor for the molecules studied was found to be over 20.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2021R1C1C2006535)supported by the Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Korea government(MSIT)(No.RS-2024-00403164)supported by the National Research Foundation of Korea grant funded by the Korea government,Ministry of Science and ICT(Development of Nanofiber Yarn Based Compound Sensor as a Comprehensive Wearable Healthcare Solution)(Grant No.RS-2024-00357296).
文摘The crystallization of ionic crystals has traditionally been explained by Gibbs's classical nucleation theory.However,recent observations of intermediate phases during nucleation suggest that the process may be more complex,necessitating new theoretical frameworks,though key empirical evidence remains elusive.In this study,we used microdroplets to investigate the crystallization of sodium halides(NaCl,NaBr,and NaI)under homogeneous nucleation conditions across a wide range of supersaturations.In the evaporating droplet,NaCl follows the classical nucleation pathway,whereas NaBr and NaI exhibit the formation of an intermediate phase prior to the nucleation of anhydrous and hydrous single crystals,respectively.Optical and computational analyses indicate that these intermediate phases are liquid crystal phases composed of contact ion pairs.These findings establish a new theoretical framework for crystal nucleation and growth and offer methods to control nucleation pathways,enabling us to achieve desired crystals regardless of specific conditions.
