查看更多>>摘要：Dual-atom catalysts(DACs)have emerged as potential catalysts for effective electroreduction of CO2 due to their high atom utilization efficiency and multiple active sites.However,the screening of DACs remains a challenge due to the large number of possible combinations,making exhaustive experimental or computational screening a daunting task.In this study,a density functional theory(DFT)-based machine learning(ML)-accelerated(DFT-ML)hybrid approach was developed to test a set of 406 dual transition metal catalysts on N-doped graphene(NG)for the electroreduction of CO2 to HCOOH.The results showed that the ML algorithms can successfully capture the relationship between the descriptors of the DACs(inputs)and the limiting potential for HCOOH generation(output).Of the four ML algorithms studied in this work,the feedforward neural network model achieved the highest prediction accuracy(the highest correlation coefficient(R2)of 0.960 and the lowest root mean square error(RMSE)of 0.319 eV on the test set)and the predicted results were verified by DFT calculations with an average abso-lute error of 0.14 eV.The DFT-ML approach identified Co-Co-NG and Ir-Fe-NG as the most active and stable electrocatalysts for the electrochemical reduction of CO2 to HCOOH.The DFT-ML hybrid approach exhibits exceptional prediction accuracy while enabling a significant reduction in screening time by an impressive 64％compared to conventional DFT-only calculations.These results demonstrate the immense potential of using ML methods to accelerate the screening and rational design of efficient catalysts for various energy and environmental applications.
查看更多>>摘要：Photoelectrochemical hydrogen evolution reaction(HER)is taken into account as an alternative to effec-tive hydrogen production,emphasizing the importance of catalysts.The magnetism of catalysts could modulate the adsorption of the H atom and further enhance the HER activity.Herein,doping the double transition metal atoms on SnS2 nanosheet(TM2@SnS2)to form the efficient magnetic catalyst is proposed to explore the spin magnetic effect on the HER performance.By performing first-principles calculations,nonmagnetic V2@SnS2 is proved to be the candidate of the HER catalyst;nevertheless,the HER activities of antiferromagnetic and ferromagnetic V2@SnS2 are relatively inferior due to the spin-induced charge redistribution.Meanwhile,machine learning analysis shows the absolute importance of the electronic structure of TM dopants and surrounding S ligands,and the HER activity could be predicted by the mod-ified band centers of S-3pz and TM-d.Furthermore,the proof-of-concept experiment has substantiated the above theoretical predictions by significantly increasing liner sweep voltammetry and photocurrent with applied magnetic field.This work provides a new avenue for uncovering the spin catalytic mecha-nism and the exploration and design of efficient HER catalysts.
查看更多>>摘要：The development of cation-disordered rocksalt(DRX)cathodes has garnered worldwide attention due to their high capacity,broad chemical space and excellent structural flexibility.However,their low intrinsic Li-ion conductivity necessitates extensive particle pulverization,typically achieved through ball-milling process,which impedes large-scale production.In this work,we present a proton-exchange assisted strategy to activate the Li-ion transport in Mn-based DRX cathodes.Short-range spinel-like ordering is observed to form within the DRX matrix after the post treatment,which significantly enhances the intrin-sic Li ion mobility.Notably,more than 280 mAh g-1 discharge capacity can be delivered at a slow rate from micrometer-sized particles with an overall disordered cation arrangement,which retains more than 150 mAh g-1 when cycled at a very high rate of 2000 mA g-1.Furthermore,we also demonstrate that the electrochemical performance of the post-treated cathodes can be further optimized by fine-tuning the reaction parameters.
查看更多>>摘要：Electronic textiles hold the merits of high conformability with the human body and natural surrounding,possessing large market demand and wide application foreground in smart wearable and portable devices.However,their further application is largely hindered by the shortage of flexible and stable power sources with multifunctional designability.Herein,a free-standing ZnHCF@CF electrode(ZnHCF grown on carbon nanotube fiber)with good mechanical deformability and high electrochemical perfor-mance for aqueous fiber-shaped calcium ion battery(FCIB)is reported.Benefiting from the unique Ca2+/H+co-insertion mechanism,the ZnHCF@CF cathode can exhibit great ion storage capability within a broadened voltage window.By pairing with a polyaniline(PANI)@CF anode,a ZnHCF@CF//PANI@CF FCIB is successfully fabricated,which exhibits a desirable volumetric energy density of 43.2 mWh cm-3 and maintains superior electrochemical properties under different deformations.Moreover,the high-energy FCIB can be harmoniously integrated with a fiber-shaped strain sensor(FSS)to achieve real-time physiological monitoring on knees during long-running,exhibiting great promise for the prac-tical application of electronic textiles.
查看更多>>摘要：Constructing a protective layer on Zn anode surface with high lattice matching to Zn(002)can facilitate preferential growth along the(002)crystal plane and suppress dendritic growth as well as interface side reactions.Whereas most of protective layers are complex and costly,making commercial applications challenging.Herein,we introduce a facile method involving the addition of CuCl2 electrolyte additives to conventional electrolyte systems,which,through rapid displacement reactions and controlled electro-chemical cycling,forms a CuZn5 alloy layer with 97.2％lattice matching to the(002)plane(CuZn5@Zn),thus regulating the(002)plane epitaxial deposition.As a result,the symmetric cells with CuZn5@Zn demonstrate an ultra-long cycle life of 3600 h at 1 mA cm-2.Under extreme conditions of high current density(20 mA cm-2)and high zinc utilization(DODZn=50％),stable cycling performance is maintained for 220 and 350 h,respectively.Furthermore,the CuZn5@Zn||NH4V4O10 full cell maintains a capacity of 120 mA h g-1 even after 10,000 cycles at a high current density of 10 A g-1.This work presents a facile and efficient strategy for constructing stable metal anode materials,with implications for the develop-ment of next-generation rechargeable batteries.
查看更多>>摘要：Accurate aging diagnosis is crucial for the health and safety management of lithium-ion batteries in elec-tric vehicles.Despite significant advancements achieved by data-driven methods,diagnosis accuracy remains constrained by the high costs of check-up tests and the scarcity of labeled data.This paper pre-sents a framework utilizing self-supervised machine learning to harness the potential of unlabeled data for diagnosing battery aging in electric vehicles during field operations.We validate our method using battery degradation datasets collected over more than two years from twenty real-world electric vehi-cles.Our analysis comprehensively addresses cell inconsistencies,physical interpretations,and charging uncertainties in real-world applications.This is achieved through self-supervised feature extraction using random short charging sequences in the main peak of incremental capacity curves.By leveraging inex-pensive unlabeled data in a self-supervised approach,our method demonstrates improvements in aver-age root mean square errors of 74.54％and 60.50％in the best and worst cases,respectively,compared to the supervised benchmark.This work underscores the potential of employing low-cost unlabeled data with self-supervised machine learning for effective battery health and safety management in real-world scenarios.
查看更多>>摘要：With the increase of people's demand,it is extremely desired for developing high-safety,wide-temperature-range and high-energy-density lithium batteries,but huge challenges are remained due to shrinkage and combustion of commonly used polyolefin separators at high temperatures,as well as narrow usable temperature range and high flammability of conventionally commercialized liquid elec-trolytes.In this work,we report a multifunctional separator mainly consisting of Zn2+-phytate coordina-tion complex nanoparticles and bacterial cellulose nanofibers,named the BZP separator,which possesses high porosity,excellent thermotolerance,good flame retardancy,abilities of anion binding and Ni2+cap-turing.Through cooperating with the fluoride-free wide-temperature-range electrolyte,Li//LiFePO4 cells not only deliver discharge capacities of 110.39 mA h g-1 and 113.25 mA h g-1 after 2200 cycles(2 C)and 1600 cycles(5 C)at 25 ℃,with capacity retentions of 76.59％and 86.09％,respectively,but also exhibit excellent cycling performance at 80 ℃ and-40 ℃.Significantly,the Li//NCM811 cell with a loading of 7.8 mg cm-2 delivers a discharge capacity of 146.64 mA h g-1 after 200 cycles at 0.5 C,with a capacity retention of 89.03％.In addition,pouch cells can work at 120 ℃ and have low flammability.
查看更多>>摘要：CO2-to-formate electrosynthesis with high selectivity and stability has been a long-sought objective.Unfortunately,most catalysts undergo structural and valence state changes due to surface oxidation dur-ing operation or storage,resulting in decreased catalytic performance.Herein,we report a efficient and stable Biln@Cu-foam electrode through the in-situ regeneration of Bi0 active sites to renew the surface activation.The electronic structure of Bi site can be regulated by introducing In,thereby enhancing the adsorption strength of*OCHO.The optimized electrode exhibits over 90％FEformate at a wide potential window(-0.9--2.2 V),and formation rate for 3.15 mM cm-1 h-1.Especially,the electrode can maintain the high performance at continuously electrolysis for more than 300 h,or for more than 50 cycles,even repeated operation and storage for more than 2 years.This work provides a promising candidate and new insight to construct industrially viable stable Bi-based catalyst for formate electrosynthesis.
查看更多>>摘要：The immerging three dimensional(3D)metal-organic framework(MOF)-reinforced composite solid-state electrolytes have attracted great interest because of the enhanced ionic conductivity and mechanical properties.However,the defective spatial arrangement of MOFs restricted by fabrication methodology leads to insufficient lithium ion transport in electrolytes.Herein,a 3D interconnected MOF framework tailored for all-solid-state electrolytes is rationally designed by a universal polydopamine(PDA)-engineered"double-sided tape"strategy.The PDA serves as a double-sided tape,firmly adhering on the special single-layer Nylon grid as well as offering uniform nucleation sites to anchor the metal nodes to ensure continuous growth of well-ordered MOFs.Benefiting from the Lewis acid feature of MOFs and its cage effect toward TFSI-,a fast and homogeneous lithium ion transport can be achieved through the internal channels within neighboring MOFs and the continuous MOFs/polymer interfaces both along the short-range circumferential boundary of Nylon fiber.The resultant composite electrolytes exhibit high lithium ion conductivity and prominent mechanical properties,rendering excellent cyclic stability whether used in coin or pouch cells.This work demonstrates a widely applicable"double-sided tape"strategy for controllable spatial arrangement of MOF nanoparticles on optional substrates,which pro-vides a scalable approach to rationally construct desired lithium ion pathways within composite electrolytes.
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