This paper demonstrates the design and fabrication of three-dimensional(3 D) hexagonally ordered microbowl arrays(MBAs) decorated with Cu In S2 nanosheets for enhanced photoelectrochemical(PEC) performance. The 3 D MB...This paper demonstrates the design and fabrication of three-dimensional(3 D) hexagonally ordered microbowl arrays(MBAs) decorated with Cu In S2 nanosheets for enhanced photoelectrochemical(PEC) performance. The 3 D MBAs are fabricated by a micro-fabrication technique. The ultrathin CuInS2 nanosheets are grown on the 3 D electrodes by solvothermal transformation of Cu film. The photocurrent density of 3 D photocathode(CuInS2@MBAs) is about two times higher than that of the planar counterpart(CuInS2@Planar). The improved PEC performance can be ascribed to the elevated light trapping ability and the increased surface area for loading photocatalysts. In addition, CdS quantum dots as cocatalysts are modified onto the Cu In S2 nanosheets to further enhance the PEC activity because the formed p-n heterojunction can accelerate the separation of photogenerated carriers. As a result, the 3 D photocathode of CuInS2/CdS@MBAs shows an optimal incident photon to current efficiency of 10% at the wavelength of400 nm. It is believed that this work can be generalized to design other hierarchical 3 D photoelectrodes for improved solar water splitting.展开更多
Real-time rapid detection of toxic gases at room temperature is particularly important for public health and environmental monitoring.Gas sensors based on conventional bulk materials often suffer from their poor surfa...Real-time rapid detection of toxic gases at room temperature is particularly important for public health and environmental monitoring.Gas sensors based on conventional bulk materials often suffer from their poor surface-sensitive sites,leading to a very low gas adsorption ability.Moreover,the charge transportation efficiency is usually inhibited by the low defect density of surface-sensitive area than that in the interior.In this work,a gas sensing structure model based on CuS quantum dots/Bi_(2)S_(3) nanosheets(CuS QDs/Bi_(2)S_(3) NSs)inspired by artificial neuron network is constructed.Simulation analysis by density functional calculation revealed that CuS QDs and Bi_(2)S_(3) NSs can be used as the main adsorption sites and charge transport pathways,respectively.Thus,the high-sensitivity sensing of NO_(2) can be realized by designing the artificial neuron-like sensor.The experimental results showed that the CuS QDs with a size of about 8 nm are highly adsorbable,which can enhance the NO_(2) sensitivity due to the rich sensitive sites and quantum size effect.The Bi_(2)S_(3) NSs can be used as a charge transfer network channel to achieve efficient charge collection and transmission.The neuron-like sensor that simulates biological smell shows a significantly enhanced response value(3.4),excellent responsiveness(18 s)and recovery rate(338 s),low theoretical detection limit of 78 ppb,and excellent selectivity for NO_(2).Furthermore,the developed wearable device can also realize the visual detection of NO2 through real-time signal changes.展开更多
Photoanodes based on In_2S_3/ZnO heterojunction nanosheet arrays(NSAs) have been fabricated by atomic layer deposition of ZnO over In_2S_3 NSAs, which were in situ grown on fluorine-doped tin oxide glasses via a facil...Photoanodes based on In_2S_3/ZnO heterojunction nanosheet arrays(NSAs) have been fabricated by atomic layer deposition of ZnO over In_2S_3 NSAs, which were in situ grown on fluorine-doped tin oxide glasses via a facile solvothermal process. The as-prepared photoanodes show dramatically enhanced performance for photoelectrochemical(PEC) water splitting, compared to single semiconductor counterparts. The optical and PEC properties of In_2S_3/ZnO NSAs have been optimized by modulating the thickness of the Zn O overlayer. After pairing with ZnO, the NSAs exhibit a broadened absorption range and an increased light absorptance over a wide wavelength region of 250–850 nm. The optimized sample of In_2S_3/ZnO-50 NSAs shows a photocurrent density of 1.642 m A cm^(-2)(1.5 V vs. RHE) and an incident photonto-current efficiency of 27.64% at 380 nm(1.23 V vs.RHE), which are 70 and 116 times higher than those of the pristine In_2S_3 NSAs, respectively. A detailed energy band edge analysis reveals the type-II band alignment of the In_2S_3/ZnO heterojunction, which enables efficient separation and collection of photogenerated carriers,especially with the assistance of positive bias potential, and then results in the significantly increased PEC activity.展开更多
In this study, hydrothermal carbonization(HTC)was applied for surface functionalization of carbon nanotubes(CNTs) in the presence of glucose and urea. The HTC process allowed the deposition of thin nitrogen-doped carb...In this study, hydrothermal carbonization(HTC)was applied for surface functionalization of carbon nanotubes(CNTs) in the presence of glucose and urea. The HTC process allowed the deposition of thin nitrogen-doped carbon layers on the surface of the CNTs. By controlling the ratio of glucose to urea, nitrogen contents of up to 1.7 wt%were achieved. The nitrogen-doped carbon nanotube-supported Pd catalysts exhibited superior electrochemical activity for ethanol oxidation relative to the pristine CNTs.Importantly, a 1.5-fold increase in the specific activity was observed for the Pd/HTC-N1.67%CNTs relative to the catalyst without nitrogen doping(Pd/HTC-CNTs). Furtherexperiments indicated that the introduction of nitrogen species on the surface of the CNTs improved the Pd(0)loading and increased the binding energy.展开更多
Biosynthesis of gold nanostructures has drawn increasing concerns because of its green and sustainable synthetic process. However, biosynthesis of gold nanoplates is still a challenge because of the expensive source a...Biosynthesis of gold nanostructures has drawn increasing concerns because of its green and sustainable synthetic process. However, biosynthesis of gold nanoplates is still a challenge because of the expensive source and difficulties of controllable formation of morphology and size. Herein, one-pot biosynthesis of gold nanoplates is proposed, in which cheap yeast was extracted as a green precursor. The morphologies and sizes of the gold nanostructures can be controlled via varying the pH value of the biomedium. In acid condition, gold nanoplates with side length from 1300 ± 200 to 300 ± 100 nm and height from 18 to 15 nm were obtained by increasing the pH value. Whereas, in neutral or basic condition, only gold nanoflowers and nanoparticles were obtained. It was determined that organic molecules, such as succinic acid, lactic acid, malic acid, and glutathione, which are generated in metabolism process, played important role in the reduction of gold ions. Besides, it was found that the gold nanoplates exhibited plasmonic property with prominent dipole infrared resonance in near-infrared region, indicating their potential in surface plasmon-enhanced applications, such as bioimaging and photothermal therapy.展开更多
As information acquisition terminals for artificial olfaction,chemiresistive gas sensors are often troubled by their cross-sensitivity,and reducing their cross-response to ambient gases has always been a difficult and...As information acquisition terminals for artificial olfaction,chemiresistive gas sensors are often troubled by their cross-sensitivity,and reducing their cross-response to ambient gases has always been a difficult and important point in the gas sensing area.Pattern recognition based on sensor array is the most conspicuous way to overcome the cross-sensitivity of gas sensors.It is crucial to choose an appropriate pattern recognition method for enhancing data analysis,reducing errors and improving system reliability,obtaining better classification or gas concentration prediction results.In this review,we analyze the sensing mechanism of crosssensitivity for chemiresistive gas sensors.We further examine the types,working principles,characteristics,and applicable gas detection range of pattern recognition algorithms utilized in gas-sensing arrays.Additionally,we report,summarize,and evaluate the outstanding and novel advancements in pattern recognition methods for gas identification.At the same time,this work showcases the recent advancements in utilizing these methods for gas identification,particularly within three crucial domains:ensuring food safety,monitoring the environment,and aiding in medical diagnosis.In conclusion,this study anticipates future research prospects by considering the existing landscape and challenges.It is hoped that this work will make a positive contribution towards mitigating cross-sensitivity in gas-sensitive devices and offer valuable insights for algorithm selection in gas recognition applications.展开更多
Leveraging big data analytics and advanced algorithms to accelerate and optimize the process of molecular and materials design, synthesis, and application has revolutionized the field of molecular and materials scienc...Leveraging big data analytics and advanced algorithms to accelerate and optimize the process of molecular and materials design, synthesis, and application has revolutionized the field of molecular and materials science, allowing researchers to gain a deeper understanding of material properties and behaviors,leading to the development of new materials that are more efficient and reliable. However, the difficulty in constructing large-scale datasets of new molecules/materials due to the high cost of data acquisition and annotation limits the development of conventional machine learning(ML) approaches. Knowledgereused transfer learning(TL) methods are expected to break this dilemma. The application of TL lowers the data requirements for model training, which makes TL stand out in researches addressing data quality issues. In this review, we summarize recent progress in TL related to molecular and materials. We focus on the application of TL methods for the discovery of advanced molecules/materials, particularly, the construction of TL frameworks for different systems, and how TL can enhance the performance of models. In addition, the challenges of TL are also discussed.展开更多
Significant challenges are posed by the limitations of gas sensing mechanisms for trace-level detection of ammonia(NH3).In this study,we propose to exploit single-atom catalytic activation and targeted adsorption prop...Significant challenges are posed by the limitations of gas sensing mechanisms for trace-level detection of ammonia(NH3).In this study,we propose to exploit single-atom catalytic activation and targeted adsorption properties to achieve highly sensitive and selective NH3 gas detection.Specifically,Ni singleatom active sites based on N,C coordination(Ni-N-C)were interfacially confined on the surface of two-dimensional(2D)MXene nanosheets(Ni-N-C/Ti_(3)C_(2)Tx),and a fully flexible gas sensor(MNPE-Ni-N-C/Ti_(3)C_(2)Tx)was integrated.The sensor demonstrates a remarkable response value to 5 ppm NH3(27.3%),excellent selectivity for NH3,and a low theoretical detection limit of 12.1 ppb.Simulation analysis by density functional calculation reveals that the Ni single-atom center with N,C coordination exhibits specific targeted adsorption properties for NH3.Additionally,its catalytic activation effect effectively reduces the Gibbs free energy of the sensing elemental reaction,while its electronic structure promotes the spill-over effect of reactive oxygen species at the gas-solid interface.The sensor has a dual-channel sensing mechanism of both chemical and electronic sensitization,which facilitates efficient electron transfer to the 2D MXene conductive network,resulting in the formation of the NH3 gas molecule sensing signal.Furthermore,the passivation of MXene edge defects by a conjugated hydrogen bond network enhances the long-term stability of MXene-based electrodes under high humidity conditions.This work achieves highly sensitive room-temperature NH3 gas detection based on the catalytic mechanism of Ni single-atom active center with N,C coordination,which provides a novel gas sensing mechanism for room-temperature trace gas detection research.展开更多
The structure of liquid water is primarily composed of three-dimensional networks of water clusters formed by hydrogen bonds,and dis-solved oxygen is one of the most important indicators for assessing water qual-ity.I...The structure of liquid water is primarily composed of three-dimensional networks of water clusters formed by hydrogen bonds,and dis-solved oxygen is one of the most important indicators for assessing water qual-ity.In this work,distilled water with different concentration of dissolved oxygen were prepared,and a clear negative correlation between the size of water clus-ters and dissolved oxygen concentration was observed.Besides,a phenomenon of rapid absorption and release of oxygen at the water interfaces was unveiled,suggesting that oxygen molecules predominantly exist at the interfaces of water clusters.Oxygen molecules can move rapidly through the interfaces among water clusters,allowing dissolved oxygen to quickly reach a saturation level at certain partial pressure of oxygen and temperature.Further exploration into the mechanism by molecular dynamics simulations of oxygen and water clusters found that oxygen molecules can only exist stably at the interfaces among water clusters.A semi-empirical formula relating the average number of water molecules in a cluster(n)to ^(17)O NMR half-peak width(W)was summarized:n=0.1 W+0.85.These findings provide a foundation for exploring the structure and properties of water.展开更多
This study presents an innovative approach to improving the performance of YOLO-v8 model for small object detection in radar images.Initially,a local histogram equalization technique was applied to the original images...This study presents an innovative approach to improving the performance of YOLO-v8 model for small object detection in radar images.Initially,a local histogram equalization technique was applied to the original images,resulting in a notable enhancement in both contrast and detail representation.Subsequently,the YOLO-v8 backbone network was augmented by incorporating convolutional kernels based on a multidimensional attention mechanism and a parallel processing strategy,which facilitated more effective feature information fusion.At the model’s head,an upsampling layer was added,along with the fusion of outputs from the shallow network,and a detection head specifically tailored for small object detection,thereby further improving accuracy.Additionally,the loss function was modified to incorporate focal-intersection over union(IoU)in conjunction with scaled-IoU,which enhanced the model’s performance.A weighting strategy was also introduced,effectively improving detection accuracy for small targets.Experimental results demonstrate that the customized model outperforms traditional approaches across various evaluation metrics,including recall,precision,F1-score,and the receiver operating characteristic(ROC)curve,validating its efficacy and innovation in small object detection within radar imagery.The results indicate a substantial improvement in accuracy compared to conventional methods such as image segmentation and standard convolutional neural networks.展开更多
Graphene-based gas/vapor sensors have attracted much attention in recent years due to their variety of structures, unique sensing performances, room-temperature working conditions, and tremendous application prospects...Graphene-based gas/vapor sensors have attracted much attention in recent years due to their variety of structures, unique sensing performances, room-temperature working conditions, and tremendous application prospects, etc.Herein, we summarize recent advantages in graphene preparation, sensor construction, and sensing properties of various graphene-based gas/vapor sensors, such as NH_3, NO_2, H_2, CO, SO_2, H_2S, as well as vapor of volatile organic compounds.The detection mechanisms pertaining to various gases are also discussed. In conclusion part, some existing problems which may hinder the sensor applications are presented. Several possible methods to solve these problems are proposed, for example, conceived solutions, hybrid nanostructures, multiple sensor arrays, and new recognition algorithm.展开更多
Human metabolite moisture detection is important in health monitoring and non-invasive diagnosis.However,ultra-sensitive quantitative extraction of respiration information in real-time remains a great challenge.Herein...Human metabolite moisture detection is important in health monitoring and non-invasive diagnosis.However,ultra-sensitive quantitative extraction of respiration information in real-time remains a great challenge.Herein,chemiresistors based on imine-linked covalent organic framework(COF)films with dual-active sites are fabricated to address this issue,which demonstrates an amplified humidity-sensing signal performance.By regulation of monomers and functional groups,these COF films can be pre-engineered to achieve high response,wide detection range,fast response,and recovery time.Under the condition of relative humidity ranging from 13 to 98%,the COFTAPB-DHTA film-based humidity sensor exhibits outstanding humidity sensing perfor-mance with an expanded response value of 390 times.Furthermore,the response values of the COF film-based sensor are highly linear to the relative humidity in the range below 60%,reflecting a quantitative sensing mechanism at the molecular level.Based on the dual-site adsorption of the(-C=N-)and(C-N)stretching vibrations,the revers-ible tautomerism induced by hydrogen bonding with water molecules is demonstrated to be the main intrinsic mechanism for this effective humidity detection.In addition,the synthesized COF films can be further exploited to effectively detect human nasal and oral breathing as well as fabric permeability,which will inspire novel designs for effective humidity-detection devices.展开更多
The application scope and future development directions of machine learning models(supervised learning, transfer learning, and unsupervised learning) that have driven energy material design are discussed.
We report the carboxylated C60 improved the survival and quality of boar sperm during liquid storage at 4°C and thus propose the use of carboxylated C60 as a novel antioxidant semen extender supplement.Our result...We report the carboxylated C60 improved the survival and quality of boar sperm during liquid storage at 4°C and thus propose the use of carboxylated C60 as a novel antioxidant semen extender supplement.Our results demonstrated that the sperm treated with 2μg mL?1 carboxylated C60 had higher motility than the control group(58.6%and 35.4%,respectively;P?0.05).Moreover,after incubation with carboxylated C60 for 10 days,acrosome integrity and mitochondrial activity of sperm increased by 18.1%and 34%,respectively,compared with that in the control group.Similarly,the antioxidation abilities and adenosine triphosphate levels in boar sperm treated with carboxylated C60 significantly increased(P?0.05)compared with those in the control group.The presence of carboxylated C60 in semen extender increases sperm motility probably by suppressing reactive oxygen species(ROS)toxicity damage.Interestingly,carboxylated C60 could protect boar sperm from oxidative stress and energy deficiency by inhibiting the ROS-induced protein dephosphorylation via the cAMP-PKA signaling pathway.In addition,the safety of carboxylated C60 as an alternative antioxidant was also comprehensively evaluated by assessing the mean litter size and number of live offspring in the carboxylated C60 treatment group.Our findings confirm carboxylated C60 as a novel antioxidant agent and suggest its use as a semen extender supplement for assisted reproductive technology in domestic animals.展开更多
The green production of hydrogen from electrocatalytic water splitting is an important base and promising direction for the future of the large-scale application of hydrogen energy.The key of green hydrogen evolution ...The green production of hydrogen from electrocatalytic water splitting is an important base and promising direction for the future of the large-scale application of hydrogen energy.The key of green hydrogen evolution depends on the development of low-cost and highly active electrocatalysts.Molybdenum carbides(MoxC),as a typical of earth-abundant transition-metal material,have accumulated great attention due to their low cost,earth abundance,electrical conductivity,similar d-band state to Pt,and regulated morphology/electronic structures.In this paper,recent researches focusing on MoxC for efficient HER in a wide pH range are summarized from respects of modulation of unique morphology,electronic structure,and electrode interface step by step.Briefly,modulation of morphology influence the apparent activity of catalyst,modulation of electronic structure of active sites by heteroatom doping and designing heterointerface boost intrinsic HER kinetics,and modulation of electrode interface via hybridization of MoxC structures with carbon materials can ensure the fast electron transfer and boost the activity.Besides the above methods discussed,perspective and challenges of designing MoxC as the substitute of Pt-based electrocatalyst for practical hydrogen generation in a wide pH range are pointed out.展开更多
基金sponsored by the National Key Research and Development Program of China (2016YFA0200800)National Natural Science Foundation of China (61804156)Shanghai Sailing Program (18YF1427800)。
文摘This paper demonstrates the design and fabrication of three-dimensional(3 D) hexagonally ordered microbowl arrays(MBAs) decorated with Cu In S2 nanosheets for enhanced photoelectrochemical(PEC) performance. The 3 D MBAs are fabricated by a micro-fabrication technique. The ultrathin CuInS2 nanosheets are grown on the 3 D electrodes by solvothermal transformation of Cu film. The photocurrent density of 3 D photocathode(CuInS2@MBAs) is about two times higher than that of the planar counterpart(CuInS2@Planar). The improved PEC performance can be ascribed to the elevated light trapping ability and the increased surface area for loading photocatalysts. In addition, CdS quantum dots as cocatalysts are modified onto the Cu In S2 nanosheets to further enhance the PEC activity because the formed p-n heterojunction can accelerate the separation of photogenerated carriers. As a result, the 3 D photocathode of CuInS2/CdS@MBAs shows an optimal incident photon to current efficiency of 10% at the wavelength of400 nm. It is believed that this work can be generalized to design other hierarchical 3 D photoelectrodes for improved solar water splitting.
基金supported by the National Natural Science Foundation of China(61971284)the Oceanic Interdisciplinary Program of Shanghai Jiao Tong University(SL2020ZD203 and SL2020MS031)+2 种基金Scientific Research Fund of Second Institute of Oceanography,Ministry of Natural Resources of P.R.China(SL2003)Shanghai Sailing Program(21YF1421400)Startup Fund for Youngman Research at Shanghai Jiao Tong University.
文摘Real-time rapid detection of toxic gases at room temperature is particularly important for public health and environmental monitoring.Gas sensors based on conventional bulk materials often suffer from their poor surface-sensitive sites,leading to a very low gas adsorption ability.Moreover,the charge transportation efficiency is usually inhibited by the low defect density of surface-sensitive area than that in the interior.In this work,a gas sensing structure model based on CuS quantum dots/Bi_(2)S_(3) nanosheets(CuS QDs/Bi_(2)S_(3) NSs)inspired by artificial neuron network is constructed.Simulation analysis by density functional calculation revealed that CuS QDs and Bi_(2)S_(3) NSs can be used as the main adsorption sites and charge transport pathways,respectively.Thus,the high-sensitivity sensing of NO_(2) can be realized by designing the artificial neuron-like sensor.The experimental results showed that the CuS QDs with a size of about 8 nm are highly adsorbable,which can enhance the NO_(2) sensitivity due to the rich sensitive sites and quantum size effect.The Bi_(2)S_(3) NSs can be used as a charge transfer network channel to achieve efficient charge collection and transmission.The neuron-like sensor that simulates biological smell shows a significantly enhanced response value(3.4),excellent responsiveness(18 s)and recovery rate(338 s),low theoretical detection limit of 78 ppb,and excellent selectivity for NO_(2).Furthermore,the developed wearable device can also realize the visual detection of NO2 through real-time signal changes.
基金sponsored by the National Natural Science Foundation of China (Nos. 51402190, 61574091)Shanghai Sailing Program (18YF1427800)the special funds for theoretical physics of the National Natural Science Foundation of China (No. 11747029)
文摘Photoanodes based on In_2S_3/ZnO heterojunction nanosheet arrays(NSAs) have been fabricated by atomic layer deposition of ZnO over In_2S_3 NSAs, which were in situ grown on fluorine-doped tin oxide glasses via a facile solvothermal process. The as-prepared photoanodes show dramatically enhanced performance for photoelectrochemical(PEC) water splitting, compared to single semiconductor counterparts. The optical and PEC properties of In_2S_3/ZnO NSAs have been optimized by modulating the thickness of the Zn O overlayer. After pairing with ZnO, the NSAs exhibit a broadened absorption range and an increased light absorptance over a wide wavelength region of 250–850 nm. The optimized sample of In_2S_3/ZnO-50 NSAs shows a photocurrent density of 1.642 m A cm^(-2)(1.5 V vs. RHE) and an incident photonto-current efficiency of 27.64% at 380 nm(1.23 V vs.RHE), which are 70 and 116 times higher than those of the pristine In_2S_3 NSAs, respectively. A detailed energy band edge analysis reveals the type-II band alignment of the In_2S_3/ZnO heterojunction, which enables efficient separation and collection of photogenerated carriers,especially with the assistance of positive bias potential, and then results in the significantly increased PEC activity.
基金financial support of the National Natural Science Foundation of China(Nos.51672045 and 11374053)Key Program of Universityindustry Collaboration from Science and Technology Department of Fujian Province(No.2015H6009)
文摘In this study, hydrothermal carbonization(HTC)was applied for surface functionalization of carbon nanotubes(CNTs) in the presence of glucose and urea. The HTC process allowed the deposition of thin nitrogen-doped carbon layers on the surface of the CNTs. By controlling the ratio of glucose to urea, nitrogen contents of up to 1.7 wt%were achieved. The nitrogen-doped carbon nanotube-supported Pd catalysts exhibited superior electrochemical activity for ethanol oxidation relative to the pristine CNTs.Importantly, a 1.5-fold increase in the specific activity was observed for the Pd/HTC-N1.67%CNTs relative to the catalyst without nitrogen doping(Pd/HTC-CNTs). Furtherexperiments indicated that the introduction of nitrogen species on the surface of the CNTs improved the Pd(0)loading and increased the binding energy.
基金supported by the National Key Research and Development Program of China(2016YFC0102700)National Natural Science Foundation of China(21171117,21271181,21473240,and 81270209)+1 种基金Medical-Engineering Crossover Fund of Shanghai Jiao Tong University(YG2015MS51 and YG2014MS66)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning
文摘Biosynthesis of gold nanostructures has drawn increasing concerns because of its green and sustainable synthetic process. However, biosynthesis of gold nanoplates is still a challenge because of the expensive source and difficulties of controllable formation of morphology and size. Herein, one-pot biosynthesis of gold nanoplates is proposed, in which cheap yeast was extracted as a green precursor. The morphologies and sizes of the gold nanostructures can be controlled via varying the pH value of the biomedium. In acid condition, gold nanoplates with side length from 1300 ± 200 to 300 ± 100 nm and height from 18 to 15 nm were obtained by increasing the pH value. Whereas, in neutral or basic condition, only gold nanoflowers and nanoparticles were obtained. It was determined that organic molecules, such as succinic acid, lactic acid, malic acid, and glutathione, which are generated in metabolism process, played important role in the reduction of gold ions. Besides, it was found that the gold nanoplates exhibited plasmonic property with prominent dipole infrared resonance in near-infrared region, indicating their potential in surface plasmon-enhanced applications, such as bioimaging and photothermal therapy.
基金supported by the National Key Research and Development Program of China(2021YFB3200400)the National Natural Science Foundation of China(62371299,62301314,and 62020106006)the China Postdoctoral Science Foundation(2023M732198).
文摘As information acquisition terminals for artificial olfaction,chemiresistive gas sensors are often troubled by their cross-sensitivity,and reducing their cross-response to ambient gases has always been a difficult and important point in the gas sensing area.Pattern recognition based on sensor array is the most conspicuous way to overcome the cross-sensitivity of gas sensors.It is crucial to choose an appropriate pattern recognition method for enhancing data analysis,reducing errors and improving system reliability,obtaining better classification or gas concentration prediction results.In this review,we analyze the sensing mechanism of crosssensitivity for chemiresistive gas sensors.We further examine the types,working principles,characteristics,and applicable gas detection range of pattern recognition algorithms utilized in gas-sensing arrays.Additionally,we report,summarize,and evaluate the outstanding and novel advancements in pattern recognition methods for gas identification.At the same time,this work showcases the recent advancements in utilizing these methods for gas identification,particularly within three crucial domains:ensuring food safety,monitoring the environment,and aiding in medical diagnosis.In conclusion,this study anticipates future research prospects by considering the existing landscape and challenges.It is hoped that this work will make a positive contribution towards mitigating cross-sensitivity in gas-sensitive devices and offer valuable insights for algorithm selection in gas recognition applications.
基金National Key R&D Program of China (No. 2021YFC2100100)Shanghai Science and Technology Project (No. 21JC1403400, 23JC1402300)。
文摘Leveraging big data analytics and advanced algorithms to accelerate and optimize the process of molecular and materials design, synthesis, and application has revolutionized the field of molecular and materials science, allowing researchers to gain a deeper understanding of material properties and behaviors,leading to the development of new materials that are more efficient and reliable. However, the difficulty in constructing large-scale datasets of new molecules/materials due to the high cost of data acquisition and annotation limits the development of conventional machine learning(ML) approaches. Knowledgereused transfer learning(TL) methods are expected to break this dilemma. The application of TL lowers the data requirements for model training, which makes TL stand out in researches addressing data quality issues. In this review, we summarize recent progress in TL related to molecular and materials. We focus on the application of TL methods for the discovery of advanced molecules/materials, particularly, the construction of TL frameworks for different systems, and how TL can enhance the performance of models. In addition, the challenges of TL are also discussed.
基金supported by the National Key Research and Development Program of China(2022YFB3205500)the National Natural Science Foundation of China(62371299,62301314 and 62101329)+2 种基金the China Postdoctoral Science Foundation(2023M732198)the Natural Science Foundation of Shanghai(23ZR1430100)supported by the Center for High-Performance Computing at Shanghai Jiao Tong University.
文摘Significant challenges are posed by the limitations of gas sensing mechanisms for trace-level detection of ammonia(NH3).In this study,we propose to exploit single-atom catalytic activation and targeted adsorption properties to achieve highly sensitive and selective NH3 gas detection.Specifically,Ni singleatom active sites based on N,C coordination(Ni-N-C)were interfacially confined on the surface of two-dimensional(2D)MXene nanosheets(Ni-N-C/Ti_(3)C_(2)Tx),and a fully flexible gas sensor(MNPE-Ni-N-C/Ti_(3)C_(2)Tx)was integrated.The sensor demonstrates a remarkable response value to 5 ppm NH3(27.3%),excellent selectivity for NH3,and a low theoretical detection limit of 12.1 ppb.Simulation analysis by density functional calculation reveals that the Ni single-atom center with N,C coordination exhibits specific targeted adsorption properties for NH3.Additionally,its catalytic activation effect effectively reduces the Gibbs free energy of the sensing elemental reaction,while its electronic structure promotes the spill-over effect of reactive oxygen species at the gas-solid interface.The sensor has a dual-channel sensing mechanism of both chemical and electronic sensitization,which facilitates efficient electron transfer to the 2D MXene conductive network,resulting in the formation of the NH3 gas molecule sensing signal.Furthermore,the passivation of MXene edge defects by a conjugated hydrogen bond network enhances the long-term stability of MXene-based electrodes under high humidity conditions.This work achieves highly sensitive room-temperature NH3 gas detection based on the catalytic mechanism of Ni single-atom active center with N,C coordination,which provides a novel gas sensing mechanism for room-temperature trace gas detection research.
基金funding support from National Natural Science Foundation of China(Project No.61574091)Wuxi River and Lake Management and Water Resources Management Center(Project No.JSXXCG2022-004).
文摘The structure of liquid water is primarily composed of three-dimensional networks of water clusters formed by hydrogen bonds,and dis-solved oxygen is one of the most important indicators for assessing water qual-ity.In this work,distilled water with different concentration of dissolved oxygen were prepared,and a clear negative correlation between the size of water clus-ters and dissolved oxygen concentration was observed.Besides,a phenomenon of rapid absorption and release of oxygen at the water interfaces was unveiled,suggesting that oxygen molecules predominantly exist at the interfaces of water clusters.Oxygen molecules can move rapidly through the interfaces among water clusters,allowing dissolved oxygen to quickly reach a saturation level at certain partial pressure of oxygen and temperature.Further exploration into the mechanism by molecular dynamics simulations of oxygen and water clusters found that oxygen molecules can only exist stably at the interfaces among water clusters.A semi-empirical formula relating the average number of water molecules in a cluster(n)to ^(17)O NMR half-peak width(W)was summarized:n=0.1 W+0.85.These findings provide a foundation for exploring the structure and properties of water.
基金supported by the Na‑tional Natural Science Foundation of China Joint Fund(No.U21B2028)the National Key R&D Program of China(No.2021YFC 2100100)the Shanghai Science and Technology Project(Nos.21JC1403400,23JC1402300).
文摘This study presents an innovative approach to improving the performance of YOLO-v8 model for small object detection in radar images.Initially,a local histogram equalization technique was applied to the original images,resulting in a notable enhancement in both contrast and detail representation.Subsequently,the YOLO-v8 backbone network was augmented by incorporating convolutional kernels based on a multidimensional attention mechanism and a parallel processing strategy,which facilitated more effective feature information fusion.At the model’s head,an upsampling layer was added,along with the fusion of outputs from the shallow network,and a detection head specifically tailored for small object detection,thereby further improving accuracy.Additionally,the loss function was modified to incorporate focal-intersection over union(IoU)in conjunction with scaled-IoU,which enhanced the model’s performance.A weighting strategy was also introduced,effectively improving detection accuracy for small targets.Experimental results demonstrate that the customized model outperforms traditional approaches across various evaluation metrics,including recall,precision,F1-score,and the receiver operating characteristic(ROC)curve,validating its efficacy and innovation in small object detection within radar imagery.The results indicate a substantial improvement in accuracy compared to conventional methods such as image segmentation and standard convolutional neural networks.
基金financial supports provided by the National Basic Research Program of China(2013CB932500)the National Natural Science Foundation of China(21171117 and 61574091)+3 种基金the Program for New Century Excellent Talents in University(NCET-12-0356)the Program of Shanghai Academic/Technology Research Leader(15XD1525200)Shanghai Jiao Tong University Agri-X Funding(Agri-X2015007)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning
文摘Graphene-based gas/vapor sensors have attracted much attention in recent years due to their variety of structures, unique sensing performances, room-temperature working conditions, and tremendous application prospects, etc.Herein, we summarize recent advantages in graphene preparation, sensor construction, and sensing properties of various graphene-based gas/vapor sensors, such as NH_3, NO_2, H_2, CO, SO_2, H_2S, as well as vapor of volatile organic compounds.The detection mechanisms pertaining to various gases are also discussed. In conclusion part, some existing problems which may hinder the sensor applications are presented. Several possible methods to solve these problems are proposed, for example, conceived solutions, hybrid nanostructures, multiple sensor arrays, and new recognition algorithm.
基金supported by the National Key Research and Development Program of China(2022YFB3205500,and 2022YFC3104700)the National Natural Science Foundation of China(62101329 and 61971284)+4 种基金the Shanghai Sailing Program(21YF1421400)the Natural Science Foundation of Shanghai(23ZR1430100)the Oceanic Interdisciplinary Program of Shanghai Jiao Tong University(SL2020ZD203,SL2021MS006 and SL2020MS031)Scientific Research Fund of Second Institute of Oceanography,Ministry of Natural Resources of P.R.China(SL2003)Startup Fund for Youngman Research at Shanghai Jiao Tong University.
文摘Human metabolite moisture detection is important in health monitoring and non-invasive diagnosis.However,ultra-sensitive quantitative extraction of respiration information in real-time remains a great challenge.Herein,chemiresistors based on imine-linked covalent organic framework(COF)films with dual-active sites are fabricated to address this issue,which demonstrates an amplified humidity-sensing signal performance.By regulation of monomers and functional groups,these COF films can be pre-engineered to achieve high response,wide detection range,fast response,and recovery time.Under the condition of relative humidity ranging from 13 to 98%,the COFTAPB-DHTA film-based humidity sensor exhibits outstanding humidity sensing perfor-mance with an expanded response value of 390 times.Furthermore,the response values of the COF film-based sensor are highly linear to the relative humidity in the range below 60%,reflecting a quantitative sensing mechanism at the molecular level.Based on the dual-site adsorption of the(-C=N-)and(C-N)stretching vibrations,the revers-ible tautomerism induced by hydrogen bonding with water molecules is demonstrated to be the main intrinsic mechanism for this effective humidity detection.In addition,the synthesized COF films can be further exploited to effectively detect human nasal and oral breathing as well as fabric permeability,which will inspire novel designs for effective humidity-detection devices.
基金supported by the National Key R&D Program of China(Grant No.2021YFC2100100)the National Natural Science Foundation of China(Grant No.21901157)+1 种基金the Shanghai Science and Technology Project of China(Grant No.21JC1403400)the SJTU Global Strategic Partnership Fund(Grant No.2020 SJTUHUJI)。
文摘The application scope and future development directions of machine learning models(supervised learning, transfer learning, and unsupervised learning) that have driven energy material design are discussed.
基金supported by the National Natural Science Foundation of China(No.31772594)the Special Fund for Agro-scientific Research in the Public Interest of China(No.200903056)the Key Project of Shanghai Municipal Agricultural Commission of China(2014-2-5).
文摘We report the carboxylated C60 improved the survival and quality of boar sperm during liquid storage at 4°C and thus propose the use of carboxylated C60 as a novel antioxidant semen extender supplement.Our results demonstrated that the sperm treated with 2μg mL?1 carboxylated C60 had higher motility than the control group(58.6%and 35.4%,respectively;P?0.05).Moreover,after incubation with carboxylated C60 for 10 days,acrosome integrity and mitochondrial activity of sperm increased by 18.1%and 34%,respectively,compared with that in the control group.Similarly,the antioxidation abilities and adenosine triphosphate levels in boar sperm treated with carboxylated C60 significantly increased(P?0.05)compared with those in the control group.The presence of carboxylated C60 in semen extender increases sperm motility probably by suppressing reactive oxygen species(ROS)toxicity damage.Interestingly,carboxylated C60 could protect boar sperm from oxidative stress and energy deficiency by inhibiting the ROS-induced protein dephosphorylation via the cAMP-PKA signaling pathway.In addition,the safety of carboxylated C60 as an alternative antioxidant was also comprehensively evaluated by assessing the mean litter size and number of live offspring in the carboxylated C60 treatment group.Our findings confirm carboxylated C60 as a novel antioxidant agent and suggest its use as a semen extender supplement for assisted reproductive technology in domestic animals.
基金financial support from Shandong Provincial Natural Science Foundation(ZR2017MB059)the National Natural Science Foundation of China(21776314)the Fundamental Research Funds for the Central Universities(18CX05016A)。
文摘The green production of hydrogen from electrocatalytic water splitting is an important base and promising direction for the future of the large-scale application of hydrogen energy.The key of green hydrogen evolution depends on the development of low-cost and highly active electrocatalysts.Molybdenum carbides(MoxC),as a typical of earth-abundant transition-metal material,have accumulated great attention due to their low cost,earth abundance,electrical conductivity,similar d-band state to Pt,and regulated morphology/electronic structures.In this paper,recent researches focusing on MoxC for efficient HER in a wide pH range are summarized from respects of modulation of unique morphology,electronic structure,and electrode interface step by step.Briefly,modulation of morphology influence the apparent activity of catalyst,modulation of electronic structure of active sites by heteroatom doping and designing heterointerface boost intrinsic HER kinetics,and modulation of electrode interface via hybridization of MoxC structures with carbon materials can ensure the fast electron transfer and boost the activity.Besides the above methods discussed,perspective and challenges of designing MoxC as the substitute of Pt-based electrocatalyst for practical hydrogen generation in a wide pH range are pointed out.
