Who/what inspires you to the field of energy and nanomaterials?My Ph.D advisor Professor Charles Lieber has been a big inspiration to me since my graduate school study.I was later influenced quite a bit by my postdoct...Who/what inspires you to the field of energy and nanomaterials?My Ph.D advisor Professor Charles Lieber has been a big inspiration to me since my graduate school study.I was later influenced quite a bit by my postdoctoral mentor Professor Paul Alivisatos.By the end of my postdoctoral study in 2005,I was also influenced by Professor Steven Chu,who is a major figure to excite me to go into the energy area.I have many on‐going collaborations with Professor Chu.展开更多
Deconfined quantum critical points(DQCPs)have been proposed as a class of continuous quantum phase transitions occurring between two ordered phases with distinct symmetry-breaking patterns,beyond the conventional fram...Deconfined quantum critical points(DQCPs)have been proposed as a class of continuous quantum phase transitions occurring between two ordered phases with distinct symmetry-breaking patterns,beyond the conventional framework of Landau-Ginzburg-Wilson(LGW)theory.At the DQCP,the system exhibits emergent gauge fields,fractionalized excitations,and enhanced symmetries.展开更多
Self-assembled monolayers(SAMs),owing to their amphiphilic nature,tend to aggregate,which impedes the formation of a dense and uniform SAM on the substrate.Additionally,the weak adsorption ability of SAMs on the indiu...Self-assembled monolayers(SAMs),owing to their amphiphilic nature,tend to aggregate,which impedes the formation of a dense and uniform SAM on the substrate.Additionally,the weak adsorption ability of SAMs on the indium tin oxide(ITO)surface and the desorption of hydroxyl(OH)from the ITO surface induced by polar solvents can lead to the formation of vacancies.Herein,a dimethylacridine-based SAM is incorporated into the perovskite precursor solution.This SAM can be extruded from the precursor solution and enriched on the bottom surface of the perovskite,filling the vacancies and in situ forming a mixed SAM with MeO-2PACz as a hole-selective layer(HSL).The in situ formed mixed SAM optimizes the energy level alignment between the HSL and the perovskite,facilitating hole extraction and alleviating the residual strain of the perovskite film.Consequently,the perovskite solar cells(PSCs),based on the mixed SAM,achieve a power conversion efficiency(PCE)of 25.69%and exhibit excellent operational stability.When this approach is applied to 1.78 eV bandgap PSC devices,it yields a PCE of 20.08%.This work presents a unique strategy for fabricating both high-quality perovskite films and superior buried interfaces,which is also applicable to wide-bandgap PSCs.展开更多
The composition and isotopic characteristics of coalbed methane(CBM), as well as the genesis of CH_(4)and CO_(2), associated geological process and migration-accumulation model of CBM in typical mid-to low-rank coal-b...The composition and isotopic characteristics of coalbed methane(CBM), as well as the genesis of CH_(4)and CO_(2), associated geological process and migration-accumulation model of CBM in typical mid-to low-rank coal-bearing basins were studied. The genesis of CBM is jointly influenced by the degree of coalification and biochemical processes, which in turn determine the composition and isotopic characteristics of CBM.Biogenic gas is extensively developed in mid-to low-rank coal-bearing basins, but its genesis varies. In the Baode area, China, and the San Juan Basin, USA, CBM is mainly secondary biogenic gas and thermogenic gas. In the Miquan area, China, CBM is characterized by primary biogenic gas. However, CBM in the Jiergalangtu area, China, Surat Basin, Australia, and Power River Basin, USA, are characterized by secondary biogenic gas. Microbial CO_(2)reduction occurs in these coal-bearing basins, but with significant gas generation by acetate fermentation in some areas of these basins. Moreover, CO_(2)in the Power River Basin, Surat Basin, and Jiergalangtu area mainly originates from microbial degradation of organic matter.However, in other basins studied, CO_(2)initially derives from coal pyrolysis and is subsequently supplemented by CO_(2)from microbial methanogenesis. The generation and isotope fractionation of CBM are affected and controlled by associated geological processes. Additionally, under the control of tectonic morphology and hydrogeological conditions, the genesis and migration-accumulation models of CBM in mid-to low-rank coal-bearing basins can be summarized into two models-the hydrodynamic active monoclinic model and the hydrodynamic differential syncline model-or a combination of the two.展开更多
Clay-type Li deposits are poised to play a pivotal role in addressing the surging global demand for Li.The McDermitt clay-type Li deposit,located in Nevada,is the largest Li deposit in the United States,with Li hosted...Clay-type Li deposits are poised to play a pivotal role in addressing the surging global demand for Li.The McDermitt clay-type Li deposit,located in Nevada,is the largest Li deposit in the United States,with Li hosted by a clay-rich sequence of smectite-dominated intervals and illite-dominated intervals,respectively.However,the occurrence of Li and the genesis of Li-bearing minerals within smectite-dominated intervals have not been thoroughly investigated in previous research.Here,we studied the mineralogy,the in-situ Li distribution,and the bonding environments of Li within the smectite intervals using a combination of instru-mental techniques including scanning electron microscope,transmission electron microscope,time-of-flight secondary ion mass spectrometry,and nuclear magnetic resonance.Our results indicate that the smectite exhibits low crystallinity characteristics of lacustrine clay authigenesis and is com-monly found tofill the interstices among volcanic minerals or envelop them;Li is mainly hosted by Mg-smectite rather than the volcanic minerals.Within the tuffaceous sediment samples,the volcanic glass has undergone a transformation,resulting in its complete disappearance and alteration into clay minerals.Owing to the octahedral sites of Mg-smectite bounded in Li,it is referred to be hectorite.We interpret that the hectorite’s precipitation occurs in a high saline-alkaline water environment,a result of McDermitt tuffdissolution.This conclusion can be supported by the coexistence of spherulitic calcite and hectorite.Overall,this study confirms hectorite as the main Li-bearing mineral and increases the understanding of the genetic model of hectorite formation in intracontinental caldera basins.展开更多
In this study,a detailed analysis of the combustion behaviors of the lithium iron phosphate(LFP)and lithium manganese oxide(LMO)batteries used in electric bicycles was conducted.This research included quantitative mea...In this study,a detailed analysis of the combustion behaviors of the lithium iron phosphate(LFP)and lithium manganese oxide(LMO)batteries used in electric bicycles was conducted.This research included quantitative measurements of the combustion duration,flame height,combustion temperature,heat release rate,and total heat release.The results indicated that LMO batteries exhibited higher combustion temperatures of 600–700°C,flame heights of 70–75 cm,a significantly higher heat release rate of40.1 k W(12 Ah),and a total heat release of 1.04 MJ(12 Ah)compared to LFP batteries with the same capacity.Based on these experimental results,a normalized total heat release(NORTHR)parameter was proposed,demonstrating good universality for batteries with different capacities.Utilizing this parameter,quantitative calculations and optimization of the extinguishing agent dosage were conducted for fires involving these two types of batteries,and the method was validated by extinguishing fires for these two types of battery packs with water-based extinguishing fluids.展开更多
电解水技术是一种生产高纯氢燃料的方法,能够增强可再生能源发电系统的消纳能力.相较于质子交换膜(PEM)电解槽,碱性(ALK)电解槽可以使用非贵金属基催化电极,拥有更高的经济效益和市场占有率.然而,由于ALK电解槽处于质子稀缺环境,阴极氢...电解水技术是一种生产高纯氢燃料的方法,能够增强可再生能源发电系统的消纳能力.相较于质子交换膜(PEM)电解槽,碱性(ALK)电解槽可以使用非贵金属基催化电极,拥有更高的经济效益和市场占有率.然而,由于ALK电解槽处于质子稀缺环境,阴极氢气演化反应(HER)动力学变得更加复杂,需要快速解离水分子提供动态质子微环境.硫化钼(MoS_(2))纳米片边缘具有合适的质子吸附和演化的活性位点,是制备HER催化剂的潜力材料.但其二维基面原子由于配位饱和,显示出较弱的质子吸附能力.如何调控MoS_(2)基面以实现水解动力与质子吸附演化动力的集成,提升MoS_(2)纳米片的碱性HER活性,具有重要的科学和应用意义.本文提出了一种Co/O双原子植入策略,精准调控双活性位点及其电子结构,实现了水解离动力和质子吸附演化动力的高效耦联.首先,利用刻蚀和电沉积的两步实验法,在MoS_(2)基面上成功引入O和Co原子;随后,结合高分辨透射电镜、高角环形暗场-扫描透射电子显微镜、同步辐射X射线吸收精细结构谱等表征分析技术,精准识别了掺杂Co/O原子的位置和配位情况:O原子替换部分S原子,Co原子占据Mo原子的上方,构建出立体凸起的“O-Co-S_(2)”配位构型.催化在线的原位表征分析结果表明:该独特的“O-Co-S_(2)”原子基序发挥着水解离与氢演化反应协同催化效应.密度泛函理论计算结果也证实了该协同机制,其中Co位点促进水的解离反应,而S位点则有助于质子的转化生成氢气.因此,Co/O掺杂MoS_(2)催化剂(Co-O@MoS_(2))表现出较好的碱性HER活性:仅需81 mV的过电位,即可达到100 mA cm^(‒2)的电流密度,Tafel斜率低至42 mV dec^(‒1),在600 mA cm^(‒2)的高电流密度测试中运行300 h活性无衰减.上述碱性HER性能不仅远高于原始的MoS_(2)纳米片,而且也领先于部分已报道结果.综上所述,本文在MoS_(2)基面上构筑了原子级协同催化活性中心,显著促进了碱性HER反应性能,为原子活化工程开发先进催化剂提供参考,在原子级基序构造、表征和功能分析方面提供借鉴.展开更多
Over the past few decades,the Internet has rapidly diffused across China.The spread of the Internet has had a profound economic and social impact on Chinese rural areas.Existing research shows that Internet access sig...Over the past few decades,the Internet has rapidly diffused across China.The spread of the Internet has had a profound economic and social impact on Chinese rural areas.Existing research shows that Internet access significantly impacts agricultural production and improves smallholder farmers’income.Beyond these,the Internet can affect other dimensions of social welfare.However,research about the impact of Internet access on dietary quality in rural China remains scarce.This study utilizes multi-period panel data from Fixed Observation Point in rural China from 2009 to 2015 to estimate the impact of Internet access on dietary quality and food consumption of rural households and conducts a causal analysis.Regression models with time and household fixed effects allow robust estimation while reducing potential issues of unobserved heterogeneity.The estimates show that Internet access has significantly increased rural household dietary quality(measured by the Chinese Diet Balance Index).Further research finds that Internet access has increased the consumption of animal products,such as aquatic and dairy products.We also examine the underlying mechanisms.Internet access improves dietary quality and food consumption mainly through increasing household income and food expenditure.These results encourage the promotion of Internet access as a valuable tool for nutritional improvements,especially in rural areas.展开更多
Surface-supported isolated atoms in single-atom catalysts(SACs)grant maximum utilization of metals in heterogeneous catalysis.Herein,we report a feasible pyrolysis strategy to synthesize Pd single atoms by thermally m...Surface-supported isolated atoms in single-atom catalysts(SACs)grant maximum utilization of metals in heterogeneous catalysis.Herein,we report a feasible pyrolysis strategy to synthesize Pd single atoms by thermally melting Pd nanoparticles on an oxygen-vacancy-rich tungsten-oxide matrix at reduction atmosphere.Near ambient pressure X-ray photoelectron spectroscopy was used to monitor the formation of zero-valence Pd single atoms and the increased metallic feature of WO_(3-x)substrate.Accordingly,the as-obtained zero-valence Pd single-atom catalyst exhibits a markedly boosted HER activity with a low overpotential(η_(10)=70 mV)at the current density of 10 mA/cm2and a small Tafel slope(b=68 mV/dec),nearly 150 mV and a 3,0-fold enhancement than those of Pd nanoparticles(η_(10)=220 mV,b=133 mV/dec)under the same conditions.In addition,quasi in situ XPS results suggest the hydrogen spillover effect is more likely to occur on Pd single atoms during the electrochemical process.Our work may pave an interesting route for the rational design of highly-efficient single-atom catalysts,and the elucidation of corresponding enhanced reaction mechanisms by the utilization of advanced characterization techniques.展开更多
We perform ^(23)Na nuclear magnetic resonance(NMR) and magnetization measurements on an S=1,quasi-2D honeycomb lattice antiferromagnet Na_(3)Ni_(2)BiO_(6).A large positive Curie-Weiss constant of 22.9 K is observed.Th...We perform ^(23)Na nuclear magnetic resonance(NMR) and magnetization measurements on an S=1,quasi-2D honeycomb lattice antiferromagnet Na_(3)Ni_(2)BiO_(6).A large positive Curie-Weiss constant of 22.9 K is observed.The NMR spectra at low fields are consistent with a zigzag magnetic order,indicating a large easy-axis anisotropy.With the field applied along the c*axis,the NMR spectra confirm the existence of a 1/3-magnetization plateau phase between 5.1 T and 7.1 T.The transition from the zigzag order to the 1/3-magnetization plateau phase is also found to be a first-order type.A monotonic decrease of the spin gap is revealed in the 1/3-magnetization plateau phase,which reaches zero at a quantum critical field H_(C)≈8.35 T before entering the fully polarized phase.These data suggest the existence of exchange frustration in the system along with strong ferromagnetic interactions,hosting the possibility for Kitaev physics.Besides,well below the ordered phase,the 1/T_(1) at high fields shows either a level off or an enhancement upon cooling below 3 K,which suggests the existence of low-energy fluctuations.展开更多
Motivated by recent experimental progress on the quasi-one-dimensional quantum magnet Ni Nb2O6, we study the spin dynamics of an S = 1 ferromagnetic Heisenberg chain with single-ion anisotropy by using a semiclassical...Motivated by recent experimental progress on the quasi-one-dimensional quantum magnet Ni Nb2O6, we study the spin dynamics of an S = 1 ferromagnetic Heisenberg chain with single-ion anisotropy by using a semiclassical molecular dynamics approach. This system undergoes a quantum phase transition from a ferromagnetic to a paramagnetic state under a transverse magnetic field, and the magnetic response reflecting this transition is well described by our semiclassical method.We show that at low temperature the transverse component of the dynamical structure factor depicts clearly the magnon dispersion, and the longitudinal component exhibits two continua associated with single-and two-magnon excitations,respectively. These spin excitation spectra show interesting temperature dependence as effects of magnon interactions. Our findings shed light on the experimental detection of spin excitations in a large class of quasi-one-dimensional magnets.展开更多
Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction ...Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction due to thermodynamic instability,which has resulted in conflicting reports within the literature regarding its role.To clarify this point,we propose a strategy consisting of modulating the electronic orbital occupancy to suppress the extensive loss of Fe atoms during the OER process.Theoretical calculations,in-situ X-ray photoelectron spectroscopy,molecular dynamics simulations,and a series of characterization showed that the stable presence of Fe not only accelerates the electron transfer process but also optimizes the reaction barriers of the oxygen evolution intermediates,promoting the phase transition of Fe_(5)Ni_(4)S_(8)to highly active catalytic species.The modulated Fe_(5)Ni_(4)S_(8)-based pre-catalysts exhibit improved OER activity and long-term durability.This study provides a novel perspective for understanding the role of Fe in the OER process.展开更多
This paper presents an optimization model for the location and capacity of electric vehicle(EV)charging stations.The model takes the multiple factors of the“vehicle-station-grid”system into account.Then,ArcScene is ...This paper presents an optimization model for the location and capacity of electric vehicle(EV)charging stations.The model takes the multiple factors of the“vehicle-station-grid”system into account.Then,ArcScene is used to couple the road and power grid models and ensure that the coupling system is strictly under the goal of minimizing the total social cost,which includes the operator cost,user charging cost,and power grid loss.An immune particle swarm optimization algorithm(IPSOA)is proposed in this paper to obtain the optimal coupling strategy.The simulation results show that the algorithm has good convergence and performs well in solving multi-modal problems.It also balances the interests of users,operators,and the power grid.Compared with other schemes,the grid loss cost is reduced by 11.1%and 17.8%,and the total social cost decreases by 9.96%and 3.22%.展开更多
Accurate prediction of electric vehicle(EV)charging loads is a foundational step in the establishment of expressway charging infrastructures.This study introduces an approach to enhance the precision of expressway EV ...Accurate prediction of electric vehicle(EV)charging loads is a foundational step in the establishment of expressway charging infrastructures.This study introduces an approach to enhance the precision of expressway EV charging load predictions.The method considers both the battery dynamic state-of-charge(SOC)and user charging decisions.Expressway network nodes were first extracted using the open Gaode Map API to establish a model that incorporates the expressway network and traffic flow fea-tures.A Gaussian mixture model is then employed to construct a SOC distribution model for mixed traffic flow.An innovative SOC dynamic translation model is then introduced to capture the dynamic characteristics of traffic flow SOC values.Based on this foun-dation,an EV charging decision model was developed which considers expressway node distinctions.EV travel characteristics are extracted from the NHTS2017 datasets to assist in constructing the model.Differentiated decision-making is achieved by utilizing improved Lognormal and Sigmoid functions.Finally,the proposed method is applied to a case study of the Lian-Huo expressway.An analysis of EV charging power converges with historical data and shows that the method accurately predicts the charging loads of EVs on expressways,thus revealing the efficacy of the proposed approach in predicting EV charging dynamics under expressway scenarios.展开更多
文摘Who/what inspires you to the field of energy and nanomaterials?My Ph.D advisor Professor Charles Lieber has been a big inspiration to me since my graduate school study.I was later influenced quite a bit by my postdoctoral mentor Professor Paul Alivisatos.By the end of my postdoctoral study in 2005,I was also influenced by Professor Steven Chu,who is a major figure to excite me to go into the energy area.I have many on‐going collaborations with Professor Chu.
基金supported by the National Natural Science Foundation of China(Grant Nos.12134020 and 12374156)the National Key Research and Development Program of China(Grant No.2023YFA1406500)。
文摘Deconfined quantum critical points(DQCPs)have been proposed as a class of continuous quantum phase transitions occurring between two ordered phases with distinct symmetry-breaking patterns,beyond the conventional framework of Landau-Ginzburg-Wilson(LGW)theory.At the DQCP,the system exhibits emergent gauge fields,fractionalized excitations,and enhanced symmetries.
基金supported by the Young Cross Team Project of CAS(No.JCTD-2021-14)the National Natural Science Foundation of China(51925206)Gusu Innovation and Entrepreneur Leading Talents(ZXL2022466)。
文摘Self-assembled monolayers(SAMs),owing to their amphiphilic nature,tend to aggregate,which impedes the formation of a dense and uniform SAM on the substrate.Additionally,the weak adsorption ability of SAMs on the indium tin oxide(ITO)surface and the desorption of hydroxyl(OH)from the ITO surface induced by polar solvents can lead to the formation of vacancies.Herein,a dimethylacridine-based SAM is incorporated into the perovskite precursor solution.This SAM can be extruded from the precursor solution and enriched on the bottom surface of the perovskite,filling the vacancies and in situ forming a mixed SAM with MeO-2PACz as a hole-selective layer(HSL).The in situ formed mixed SAM optimizes the energy level alignment between the HSL and the perovskite,facilitating hole extraction and alleviating the residual strain of the perovskite film.Consequently,the perovskite solar cells(PSCs),based on the mixed SAM,achieve a power conversion efficiency(PCE)of 25.69%and exhibit excellent operational stability.When this approach is applied to 1.78 eV bandgap PSC devices,it yields a PCE of 20.08%.This work presents a unique strategy for fabricating both high-quality perovskite films and superior buried interfaces,which is also applicable to wide-bandgap PSCs.
基金supported by the National Natural Science Foundation of China(No.42272200)The Science and Technology Major Project of China National Petroleum Corporation(No.2023ZZ18-03)+1 种基金The Science and Technology Major Project of Changqing Oilfield(No.2023DZZ01)The Technology project of Huaneng Group Headquarters(Medium-deep Low-Rank Coalbed Methane Resource Potential Evaluation and Key Development Technologies of Zhalainuoer Coalfield,No.HNKJ23-H51).
文摘The composition and isotopic characteristics of coalbed methane(CBM), as well as the genesis of CH_(4)and CO_(2), associated geological process and migration-accumulation model of CBM in typical mid-to low-rank coal-bearing basins were studied. The genesis of CBM is jointly influenced by the degree of coalification and biochemical processes, which in turn determine the composition and isotopic characteristics of CBM.Biogenic gas is extensively developed in mid-to low-rank coal-bearing basins, but its genesis varies. In the Baode area, China, and the San Juan Basin, USA, CBM is mainly secondary biogenic gas and thermogenic gas. In the Miquan area, China, CBM is characterized by primary biogenic gas. However, CBM in the Jiergalangtu area, China, Surat Basin, Australia, and Power River Basin, USA, are characterized by secondary biogenic gas. Microbial CO_(2)reduction occurs in these coal-bearing basins, but with significant gas generation by acetate fermentation in some areas of these basins. Moreover, CO_(2)in the Power River Basin, Surat Basin, and Jiergalangtu area mainly originates from microbial degradation of organic matter.However, in other basins studied, CO_(2)initially derives from coal pyrolysis and is subsequently supplemented by CO_(2)from microbial methanogenesis. The generation and isotope fractionation of CBM are affected and controlled by associated geological processes. Additionally, under the control of tectonic morphology and hydrogeological conditions, the genesis and migration-accumulation models of CBM in mid-to low-rank coal-bearing basins can be summarized into two models-the hydrodynamic active monoclinic model and the hydrodynamic differential syncline model-or a combination of the two.
基金This work was financially supported by the National Natural Science Foundation of China(Grant Nos.92162214,41773015,and U1812402)the Key Research and Development Program of Yunnan Province(202103AQ100003).
文摘Clay-type Li deposits are poised to play a pivotal role in addressing the surging global demand for Li.The McDermitt clay-type Li deposit,located in Nevada,is the largest Li deposit in the United States,with Li hosted by a clay-rich sequence of smectite-dominated intervals and illite-dominated intervals,respectively.However,the occurrence of Li and the genesis of Li-bearing minerals within smectite-dominated intervals have not been thoroughly investigated in previous research.Here,we studied the mineralogy,the in-situ Li distribution,and the bonding environments of Li within the smectite intervals using a combination of instru-mental techniques including scanning electron microscope,transmission electron microscope,time-of-flight secondary ion mass spectrometry,and nuclear magnetic resonance.Our results indicate that the smectite exhibits low crystallinity characteristics of lacustrine clay authigenesis and is com-monly found tofill the interstices among volcanic minerals or envelop them;Li is mainly hosted by Mg-smectite rather than the volcanic minerals.Within the tuffaceous sediment samples,the volcanic glass has undergone a transformation,resulting in its complete disappearance and alteration into clay minerals.Owing to the octahedral sites of Mg-smectite bounded in Li,it is referred to be hectorite.We interpret that the hectorite’s precipitation occurs in a high saline-alkaline water environment,a result of McDermitt tuffdissolution.This conclusion can be supported by the coexistence of spherulitic calcite and hectorite.Overall,this study confirms hectorite as the main Li-bearing mineral and increases the understanding of the genetic model of hectorite formation in intracontinental caldera basins.
基金supported by the New Energy Vehicle Power Battery Life Cycle Testing and Verification Public Service Platform Project[2022-235-224]the Beijing Science and Technology Planning Project[Z221100005222004]+1 种基金the Key Technologies Research and Development Program[2021YFB2012504]the Beijing Goldenbridge Project[ZZ2023002]。
文摘In this study,a detailed analysis of the combustion behaviors of the lithium iron phosphate(LFP)and lithium manganese oxide(LMO)batteries used in electric bicycles was conducted.This research included quantitative measurements of the combustion duration,flame height,combustion temperature,heat release rate,and total heat release.The results indicated that LMO batteries exhibited higher combustion temperatures of 600–700°C,flame heights of 70–75 cm,a significantly higher heat release rate of40.1 k W(12 Ah),and a total heat release of 1.04 MJ(12 Ah)compared to LFP batteries with the same capacity.Based on these experimental results,a normalized total heat release(NORTHR)parameter was proposed,demonstrating good universality for batteries with different capacities.Utilizing this parameter,quantitative calculations and optimization of the extinguishing agent dosage were conducted for fires involving these two types of batteries,and the method was validated by extinguishing fires for these two types of battery packs with water-based extinguishing fluids.
文摘电解水技术是一种生产高纯氢燃料的方法,能够增强可再生能源发电系统的消纳能力.相较于质子交换膜(PEM)电解槽,碱性(ALK)电解槽可以使用非贵金属基催化电极,拥有更高的经济效益和市场占有率.然而,由于ALK电解槽处于质子稀缺环境,阴极氢气演化反应(HER)动力学变得更加复杂,需要快速解离水分子提供动态质子微环境.硫化钼(MoS_(2))纳米片边缘具有合适的质子吸附和演化的活性位点,是制备HER催化剂的潜力材料.但其二维基面原子由于配位饱和,显示出较弱的质子吸附能力.如何调控MoS_(2)基面以实现水解动力与质子吸附演化动力的集成,提升MoS_(2)纳米片的碱性HER活性,具有重要的科学和应用意义.本文提出了一种Co/O双原子植入策略,精准调控双活性位点及其电子结构,实现了水解离动力和质子吸附演化动力的高效耦联.首先,利用刻蚀和电沉积的两步实验法,在MoS_(2)基面上成功引入O和Co原子;随后,结合高分辨透射电镜、高角环形暗场-扫描透射电子显微镜、同步辐射X射线吸收精细结构谱等表征分析技术,精准识别了掺杂Co/O原子的位置和配位情况:O原子替换部分S原子,Co原子占据Mo原子的上方,构建出立体凸起的“O-Co-S_(2)”配位构型.催化在线的原位表征分析结果表明:该独特的“O-Co-S_(2)”原子基序发挥着水解离与氢演化反应协同催化效应.密度泛函理论计算结果也证实了该协同机制,其中Co位点促进水的解离反应,而S位点则有助于质子的转化生成氢气.因此,Co/O掺杂MoS_(2)催化剂(Co-O@MoS_(2))表现出较好的碱性HER活性:仅需81 mV的过电位,即可达到100 mA cm^(‒2)的电流密度,Tafel斜率低至42 mV dec^(‒1),在600 mA cm^(‒2)的高电流密度测试中运行300 h活性无衰减.上述碱性HER性能不仅远高于原始的MoS_(2)纳米片,而且也领先于部分已报道结果.综上所述,本文在MoS_(2)基面上构筑了原子级协同催化活性中心,显著促进了碱性HER反应性能,为原子活化工程开发先进催化剂提供参考,在原子级基序构造、表征和功能分析方面提供借鉴.
基金This study was supported in part by the National Natural Science Foundation of China(71973136 and 72061147002)the 2115 Talent Development Program of China Agricultural University.
文摘Over the past few decades,the Internet has rapidly diffused across China.The spread of the Internet has had a profound economic and social impact on Chinese rural areas.Existing research shows that Internet access significantly impacts agricultural production and improves smallholder farmers’income.Beyond these,the Internet can affect other dimensions of social welfare.However,research about the impact of Internet access on dietary quality in rural China remains scarce.This study utilizes multi-period panel data from Fixed Observation Point in rural China from 2009 to 2015 to estimate the impact of Internet access on dietary quality and food consumption of rural households and conducts a causal analysis.Regression models with time and household fixed effects allow robust estimation while reducing potential issues of unobserved heterogeneity.The estimates show that Internet access has significantly increased rural household dietary quality(measured by the Chinese Diet Balance Index).Further research finds that Internet access has increased the consumption of animal products,such as aquatic and dairy products.We also examine the underlying mechanisms.Internet access improves dietary quality and food consumption mainly through increasing household income and food expenditure.These results encourage the promotion of Internet access as a valuable tool for nutritional improvements,especially in rural areas.
基金the support from the National Key R&D Program of China(No.2022YFA1503801)the National Natural Science Foundation of China(No.22172190,No.22202232 and No.22109171)。
文摘Surface-supported isolated atoms in single-atom catalysts(SACs)grant maximum utilization of metals in heterogeneous catalysis.Herein,we report a feasible pyrolysis strategy to synthesize Pd single atoms by thermally melting Pd nanoparticles on an oxygen-vacancy-rich tungsten-oxide matrix at reduction atmosphere.Near ambient pressure X-ray photoelectron spectroscopy was used to monitor the formation of zero-valence Pd single atoms and the increased metallic feature of WO_(3-x)substrate.Accordingly,the as-obtained zero-valence Pd single-atom catalyst exhibits a markedly boosted HER activity with a low overpotential(η_(10)=70 mV)at the current density of 10 mA/cm2and a small Tafel slope(b=68 mV/dec),nearly 150 mV and a 3,0-fold enhancement than those of Pd nanoparticles(η_(10)=220 mV,b=133 mV/dec)under the same conditions.In addition,quasi in situ XPS results suggest the hydrogen spillover effect is more likely to occur on Pd single atoms during the electrochemical process.Our work may pave an interesting route for the rational design of highly-efficient single-atom catalysts,and the elucidation of corresponding enhanced reaction mechanisms by the utilization of advanced characterization techniques.
基金Project supported by the National Key R&D Program of China (Grant Nos. 2023YFA1406500, 2022YFA1402700, and 2021YFA1400400)the National Natural Science Foundation of China (Grant Nos. 12134020, 12374156, 12104503,12061131004, 12225407, and 12074174)。
文摘We perform ^(23)Na nuclear magnetic resonance(NMR) and magnetization measurements on an S=1,quasi-2D honeycomb lattice antiferromagnet Na_(3)Ni_(2)BiO_(6).A large positive Curie-Weiss constant of 22.9 K is observed.The NMR spectra at low fields are consistent with a zigzag magnetic order,indicating a large easy-axis anisotropy.With the field applied along the c*axis,the NMR spectra confirm the existence of a 1/3-magnetization plateau phase between 5.1 T and 7.1 T.The transition from the zigzag order to the 1/3-magnetization plateau phase is also found to be a first-order type.A monotonic decrease of the spin gap is revealed in the 1/3-magnetization plateau phase,which reaches zero at a quantum critical field H_(C)≈8.35 T before entering the fully polarized phase.These data suggest the existence of exchange frustration in the system along with strong ferromagnetic interactions,hosting the possibility for Kitaev physics.Besides,well below the ordered phase,the 1/T_(1) at high fields shows either a level off or an enhancement upon cooling below 3 K,which suggests the existence of low-energy fluctuations.
基金Project supported by the National Key R&D Program of China (Grant No. 2023YFA1406500)the National Natural Science Foundation of China (Grant Nos. 12334008, 12174441,12134020, and 12374156)。
文摘Motivated by recent experimental progress on the quasi-one-dimensional quantum magnet Ni Nb2O6, we study the spin dynamics of an S = 1 ferromagnetic Heisenberg chain with single-ion anisotropy by using a semiclassical molecular dynamics approach. This system undergoes a quantum phase transition from a ferromagnetic to a paramagnetic state under a transverse magnetic field, and the magnetic response reflecting this transition is well described by our semiclassical method.We show that at low temperature the transverse component of the dynamical structure factor depicts clearly the magnon dispersion, and the longitudinal component exhibits two continua associated with single-and two-magnon excitations,respectively. These spin excitation spectra show interesting temperature dependence as effects of magnon interactions. Our findings shed light on the experimental detection of spin excitations in a large class of quasi-one-dimensional magnets.
基金financially supported by the Scientific and Technological Development Program of Jilin Province(20220201138GX)the support of the National Key R&D Program of China(No.2022YFA1503801)+1 种基金CAS Project for Young Scientists in Basic Research(No.YSBR-022)the Young Cross Team Project of CAS(No.JCTD-2021-14)。
文摘Ni-Fe-based catalysts are considered to be among the most active catalysts for the oxygen evolution reaction(OER)under alkaline conditions,with Fe playing a crucial role.However,Fe leaching occurs during the reaction due to thermodynamic instability,which has resulted in conflicting reports within the literature regarding its role.To clarify this point,we propose a strategy consisting of modulating the electronic orbital occupancy to suppress the extensive loss of Fe atoms during the OER process.Theoretical calculations,in-situ X-ray photoelectron spectroscopy,molecular dynamics simulations,and a series of characterization showed that the stable presence of Fe not only accelerates the electron transfer process but also optimizes the reaction barriers of the oxygen evolution intermediates,promoting the phase transition of Fe_(5)Ni_(4)S_(8)to highly active catalytic species.The modulated Fe_(5)Ni_(4)S_(8)-based pre-catalysts exhibit improved OER activity and long-term durability.This study provides a novel perspective for understanding the role of Fe in the OER process.
基金supported by the Major Science and Technology Projects in Gansu Province(2023ZDGA005).
文摘This paper presents an optimization model for the location and capacity of electric vehicle(EV)charging stations.The model takes the multiple factors of the“vehicle-station-grid”system into account.Then,ArcScene is used to couple the road and power grid models and ensure that the coupling system is strictly under the goal of minimizing the total social cost,which includes the operator cost,user charging cost,and power grid loss.An immune particle swarm optimization algorithm(IPSOA)is proposed in this paper to obtain the optimal coupling strategy.The simulation results show that the algorithm has good convergence and performs well in solving multi-modal problems.It also balances the interests of users,operators,and the power grid.Compared with other schemes,the grid loss cost is reduced by 11.1%and 17.8%,and the total social cost decreases by 9.96%and 3.22%.
基金supported by the Unveiling and Leading Projects of Gansu Provincial Department of Transportation(JT-JJ-2023-008).
文摘Accurate prediction of electric vehicle(EV)charging loads is a foundational step in the establishment of expressway charging infrastructures.This study introduces an approach to enhance the precision of expressway EV charging load predictions.The method considers both the battery dynamic state-of-charge(SOC)and user charging decisions.Expressway network nodes were first extracted using the open Gaode Map API to establish a model that incorporates the expressway network and traffic flow fea-tures.A Gaussian mixture model is then employed to construct a SOC distribution model for mixed traffic flow.An innovative SOC dynamic translation model is then introduced to capture the dynamic characteristics of traffic flow SOC values.Based on this foun-dation,an EV charging decision model was developed which considers expressway node distinctions.EV travel characteristics are extracted from the NHTS2017 datasets to assist in constructing the model.Differentiated decision-making is achieved by utilizing improved Lognormal and Sigmoid functions.Finally,the proposed method is applied to a case study of the Lian-Huo expressway.An analysis of EV charging power converges with historical data and shows that the method accurately predicts the charging loads of EVs on expressways,thus revealing the efficacy of the proposed approach in predicting EV charging dynamics under expressway scenarios.
