High energy density in ultra-thick and flexible electrodes enabled by designed conductive agent/binder composite

Thick electrodes can increase incorporation of active electrode materials by diminishing the proportion of inactive constituents,improving the overall energy density of batteries.However,thick electrodes fabricated using the conventional slurry casting approach frequently exhibit an exacerbated accumulation of carbon additives and binders on their surfaces,invariably leading to compromised electrochemical properties.In this study,we introduce a designed conductive agent/binder composite synthesized from carbon nanotube and polytetrafluoroethylene.This agent/binder composite facilitates production of dry-process-prepared ultra-thick electrodes endowed with a three-dimensional and uniformly distributed percolative architecture,ensuring superior electronic conductivity and remarkable mechanical resilience.Using this approach,ultra-thick LiCoO_(2)(LCO) electrodes demonstrated superior cycling performance and rate capabilities,registering an impressive loading capacity of up to 101.4 mg/cm^(2),signifying a 242% increase in battery energy density.In another analytical endeavor,time-of-flight secondary ion mass spectroscopy was used to clarify the distribution of cathode electrolyte interphase(CEI) in cycled LCO electrodes.The results provide unprecedented evidence explaining the intricate correlation between CEI generation and carbon distribution,highlighting the intrinsic advantages of the proposed dry-process approach in fine-tu ning the CEI,with excellent cycling performance in batteries equipped with ultra-thick electrodes.

Molecular Reactivity and Interface Stability Modification in In-Situ Gel Electrolyte for High Performance Quasi-Solid-State Lithium Metal Batteries

Quasi-solid-state lithium metal battery is a promising candidate for next generation high energy density and high safety power supply.Despite intensive efforts on electrolytes,uncontrolled interfacial reactions on lithium with electrolyte and patchy interfacial contacts still hinder its practical process.Herein,we bring in rationally designed F contained groups into polymer skeleton via in-situ gelation for the first time to establish quasi-solid-state battery.This method achieves a capacity retention of 90%after 1000 cycles at 0.5C with LiFePO_(4)cathodes.The interface constructed by polymer skeleton and reaction with–CF_(3)lead to the predicted solid electrolyte interface species with high stability.Furthermore,we optimize molecular reactivity and interface stability with regulating F contained end groups in the polymer.Comparisons on different structures reveal that high performance solid stable lithium metal batteries rely on chemical modification as well as stable polymer skeleton,which is more critical to construct robust and steady SEI with uniform lithium deposition.New approach with functional groups regulation proposes a more stable cycling process with a capacity retention of 94.2%at 0.5C and 87.6%at 1C after 1000 cycles with LiFePO_(4) cathodes,providing new insights for the practical development of quasi-solid-state lithium metal battery.

Structural regulation chemistry of lithium-ion solvation in nonflammable phosphate-based electrolytes for high interfacial compatibility with graphite anode

With the booming development of lithium-ion batteries,safety has become one of the most primary focuses of current researches.Although there are various approaches to enhance the safety of lithiumion batteries,phosphate-based electrolyte holds the greatest potential for practical application due to their non-flammability.Nonetheless,its compatibility issue with the graphite anode remains a significant obstacle to its widespread use.Herein,an effective method is proposed to improve the compatibility of electrolyte with graphite(Gr)anode by rationally adjusting the proportion of lithium salt and solvent components to optimize the Li^(+)solvation structure.By slightly increasing the Li^(+)/triethyl phosphate(TEP)ratio,TEP alone cannot fully occupy the inner solvation sheath and therefore less polar ethylene carbonate(EC)has to be recruited,and the solvation structure gradually changes from Li^(+)–[TEP]_(4)to Li^(+)–[TEP]_(3)[EC]with the coexistence of EC and TEP.Simultaneously,EC molecules in the Li^(+)–[TEP]_(3)[EC]could be preferentially reduced on graphite compared to the TEP molecules,resulting in the formation of a uniform and durable solid-electrolyte interphase(SEI)layer.Benefiting from the optimized phosphate-based electrolyte,the Gr|Li battery exhibits a capacity retention rate of 96.8%after stable cycling at 0.5 C for 470 cycles which shows a longer cycle life than the battery with carbonate electrolyte(cycling at 0.5 C for 450 cycles).Therefore,this work provides the guidance for designing a non-flammable phosphate-based electrolyte for high-safety and long cycling-life lithium-ion batteries.

Soil NOx Emission Prediction via Recurrent Neural Networks

This paper presents designing sequence-to-sequence recurrent neural network(RNN)architectures for a novel study to predict soil NOx emissions,driven by the imperative of understanding and mitigating environmental impact.The study utilizes data collected by the Environmental Protection Agency(EPA)to develop two distinct RNN predictive models:one built upon the long-short term memory(LSTM)and the other utilizing the gated recurrent unit(GRU).These models are fed with a combination of historical and anticipated air temperature,air moisture,and NOx emissions as inputs to forecast future NOx emissions.Both LSTM and GRU models can capture the intricate pulse patterns inherent in soil NOx emissions.Notably,the GRU model emerges as the superior performer,surpassing the LSTM model in predictive accuracy while demonstrating efficiency by necessitating less training time.Intriguingly,the investigation into varying input features reveals that relying solely on past NOx emissions as input yields satisfactory performance,highlighting the dominant influence of this factor.The study also delves into the impact of altering input series lengths and training data sizes,yielding insights into optimal configurations for enhanced model performance.Importantly,the findings promise to advance our grasp of soil NOx emission dynamics,with implications for environmental management strategies.Looking ahead,the anticipated availability of additional measurements is poised to bolster machine-learning model efficacy.Furthermore,the future study will explore physical-based RNNs,a promising avenue for deeper insights into soil NOx emission prediction.

Silicon micropillar electrodes of lithiumion batteries used for characterizing electrolyte additives

The 100 crystal-oriented silicon micropillar array platforms were prepared by microfabrication processes for the purpose of electrolyte additive identification. The silicon micropillar array platform was used for the study of fluorinated vinyl carbonate(FEC), vinyl ethylene carbonate(VEC), ethylene sulfite(ES), and vinyl carbonate(VC) electrolyte additives in the LiPF_6 dissolved in a mixture of ethylene carbonate and diethyl carbonate electrolyte system using charge/discharge cycles, electrochemical impedance spectroscopy, cyclic voltammetry, scanning electron microscopy, and x-ray photoelectron spectroscopy. The results show that the silicon pillar morphology displays cross-shaped expansion after lithiation/delithiation, the inorganic lithium salt keeps the silicon pillar morphology intact, and the organic lithium salt content promotes a rougher silicon pillar surface. The presence of poly-(VC) components on the surface of FEC and VC electrodes allows the silicon pillar to accommodate greater volume expansion while remaining intact. This work provides a standard, fast, and effective test method for the performance analysis of electrolyte additives and provides guidance for the development of new electrolyte additives.

Calibration of the superconducting gravimeter based on a cold atom absolute gravimeter at NIM

The scale factor of a superconducting gravimeter（SG） is usually calibrated by using simultaneous and co-located gravity measurements with the FG5-type absolute gravimeter（AG）. In this paper, another new kind of absolute gravimetercold atom gravimeter（CAG） is first reported to calibrate the SG. Five-day side-by-side gravity measurements have been carried out by using our CAG（NIM-AGRb-1） to calibrate the SG（iGrav-012） located at Changping Campus of the National Institute of Metrology（NIM） of China. A weighted least-squares method is applied to determine the scale factor and the result is given as（-928.01 ± 0.73） nm·s;·V;with a precision of 0.79‰. We have demonstrated that a calibration precision of 1‰ level can be achieved after 3 days of parallel observations at spring tide. The obtained calibration results are then compared with the previous calibration by FG5 X-249, which shows that the calibration precision obtained by using NIM-AGRb-1 was slightly higher than FG5 X-249 with the same time interval. The factors affecting the calibration precision are analyzed in the calibrations by means of different AGs. Finally, several calibration experiments for SG iGrav-012 are discussed. The final scale factor is estimated as（-927.58 ± 0.36） nm·s;·V;with an accuracy of 0.39‰. Our main results demonstrate that the CAGs can be used for high-precision calibrations of SGs.

自组装制备高路易斯碱度和优异电子特性的3D碳网络电催化剂在碱性金属-空气电池中的应用（英文）

碳材料具有良好的稳定性,且容易在碳晶格形成缺陷,具备一定的催化活性,因此碳材料作为一种可替代贵金属电催化剂的材料是催化领域的研究热点.通过杂原子的引进,可以改变相应碳原子的结构特性,进而提升其催化活性.其中N的电负性强于C,N元素的引入影响C的原子结构使其作为活性位点催化氧气还原.S元素与C元素的电负性相近,S掺杂的过程中会增大C原子周围的自旋电子密度,从而增大其对0_2的吸附能力,提高其催化活性.两种作用方式不同的掺杂元素之间会形成一种协同效应,进而提高碳材料的催化活性.本文采用三聚氰胺的溶剂法制备了三维结构N,S共掺杂碳网络.三聚氰胺和十二烷基苯磺钠在溶液中分布以正、负离子团存在,以其在二氧化硅模板外形成的缔合物作为前驱体,直接制备活性材料.采用扫描电子显微镜(SEM),X射线光电子能谱(XPS),拉曼光谱(Raman)等手段研究了材料的合成过程及具有优良催化活性的原因.SEM,TEM和BET结果表明材料具有良好的孔道结构和较高的比表面积(385.09 m^2/g).Raman和XPS分析证明了N,S共掺杂后的材料中碳晶格的缺陷程度明显增大,而其中存在的吡啶N位于石墨平面的边缘部位,与两个C原子相连,这种N影响了相连C的路易斯碱度,改善了其吸附氧气能力.同时,由DFT计算结果可知,噻吩S的存在可以改变相连C原子的自旋电子密度,与掺杂的N原子形成有效的防协同作用,提高其对氧气的催化活性.相应的电催化性能测试表明,在0.1 mol/L KOH溶液中,共掺杂材料的起始电位为-0.08 V,优于其他两种对比材料,与商用Pt/C催化剂相近.N,S掺杂显著提高了碳材料的催化性能,共掺杂材料表现出了较单一N掺杂更为优异的催化性能.在铝空气电池放电过程中,以共掺杂碳材料制备的空气电极具有优良的放电性能,在50 mA/cm^2的电流密度下放电,电压达到1.34 V.共掺杂材料良好的催化活性显著减少了空气电极处的极化,提高了铝空气电池的放电电压.这种制备方法可为具有此类溶液特性的物质提供参考,用以合成相应的掺杂碳材料作为催化剂材料和电极材料。

Coexistence of Charge Order and Antiferromagnetic Order in an Extended Periodic Anderson Model

The competition between the RKKY interaction and the Kondo effect leads to a magnetic phase transition,which occurs ubiquitously in heavy fermion materials.However,there are more and more experimental evidences indicating that the valence fluctuation plays an essential role in the Ce-and Y-based compounds.We study an extended periodic Anderson model(EPAM)which includes the onsite Coulomb repulsion Ucf between the localized electrons and conduction electrons.By employing the density matrix embedding theory,we investigate the EPAM in the symmetric case at half filling.By fixing the onsite Coulomb repulsion U of the localized electrons to an intermediate value,the interplay between the RKKY interaction,the Kondo effect and the Coulomb repulsion Ucf brings rich physics.We find three different phases,the antiferromagnetic phase,the charge order phase and paramagnetic phase.When the hybridization strength V between the localized orbital and the conduction orbital is small,the Kondo effect is weak so that the AF phase and the CO phase are present.The phase transition between the two long-range ordered phase is of first order.We also find a coexistence region between the two phases.As V increases,the Kondo effect becomes stronger,and the paramagnetic phase appears between the other two phases.

Detecting the vector of nanoscale light field with atomic defect

Modulation of a vector light field has played an important role in the research of nanophotonics.However,it is still a great challenge to accurately measure the three-dimensional vector distribution at nanoscale.Here,based on the interaction between the light field and atomic-sized nitrogen-vacancy(NV)color center in diamonds,we demonstrate an efficient method for vectorial mapping of the light-field distribution at nanoscale.Single NV centers with different but well-defined symmetry axes are selected and then interact with the same tightly focused light field.The excitation of a single NV center is related to the angle between the NV center axis and the polarization of the light field.Then the fluorescence patterns of different NV centers provide the information on the vectorial light field distribution.Subsequently analyzing the fluorescence patterns with the help of a deep neural network,the intensity and phase of the light-field vectorial components are fully reconstructed with nanometer resolution.The experimental results are in agreement with theoretical calculations.It demonstrates that our method can help to study light–matter interaction at nanoscale and extend the application of vector light fields in research on nanophotonics.

Boosting reversible anionic redox reaction with Li/Cu dual honeycomb centers

The anionic redox reaction(ARR)is a promising charge contributor to improve the reversible capacity of layeredoxide cathodes for Na-ion batteries;however,some practical bottlenecks still need to be eliminated,including a low capacity retention,large voltage hysteresis,and low rate capability.Herein,we proposed a high-Na content honeycomb-ordered cathode,P2–Na_(5/6)[Li_(1/6)Cu_(1/6)Mn_(2/3)]O_(2)(P2-NLCMO),with combined cationic/anionic redox.Neutron powder diffraction and X-ray diffraction of P2-NLCMO suggested P2-type stacking with rarely found P6322 symmetry.In addition,advanced spectroscopy techniques and density functional theory calculations confirmed the synergistic stabilizing relationship between the Li/Cu dual honeycomb centers,achieving fully active Cu^(3+)/Cu^(2+) redox and stabilized ARR with interactively suppressed local distortion.With a meticulously regulated charge/discharge protocol,both the cycling and rate capability of P2-NLCMO were significantly.

Participation in the absolute gravity comparison with a compact cold atom gravimeter

The first Asia-Pacific Comparison of Absolute Gravimeters(APMP.M.G-K1) was organized by the National Institute of Metrology(NIM) of China from December 21, 2015 to March 25, 2016 in Changping, Beijing. Our compact cold atom gravimeter(CCAG) was transported from Hangzhou to Beijing with a long distance of about1200 km to participate in this comparison. The CCAG is the only one, to the best of our knowledge, that is based on the principle of atom interferometry among all the instruments. Absolute gravity in the indicated three test sites has been measured as requested by the organizer. The sensitivity of our CCAG is estimated to be90 μGal∕Hz p, even when the measurements are carried out without any vibration isolation. Besides, the accuracy of this gravimeter has been evaluated to be about 19 μGal by considering the significant system errors.Our results show a good agreement with the given reference value.

Role ofδ-ferrite in fatigue crack growth of AISI 316 austenitic stainless steel

FF sample(nearly free ofδ-ferrite)and CF sample(containing∼4%δ-ferrite)were prepared from the AISI 316 austenitic stainless steel plate to elucidate the role ofδ-ferrite in the fatigue crack growth under the solution treated and accelerated aged conditions.It is found that the fatigue crack growth resistance of the CF sample is higher than the FF sample under the solution treated condition.However,a significant deterioration of the fatigue crack growth resistance is observed in the CF sample while little variation is found in the FF sample after accelerated aging treatment at 750°C for 10 h.In the solution treated condition,deflected crack growth path is present when the main crack encounters theδ-ferrite in the CF sample due to the differences in the fatigue responses between austenite andδ-ferrite.The measured growth rate of the deflected crack is significantly slower than that of the flat crack of the same length.After the accelerated aging treatment,microcracks are produced at the M_(23)C_(6)/δinterface due to the strain incompatibility between M_(23)C_(6) and retainedδ-ferrite when the decomposedδ-ferrite is subject to plastic deformation in the crack tip plastic zone.The preexisting microcracks in the front of crack tip provide a viable path for crack propagation,resulting in the relatively flat crack path.