Rational design of carbon skeleton interfaces for highly reversible sodium metal battery anodes

Sodium metal batteries(SMBs)have attracted increasing attention over time due to their abundance of sodium resources and low cost.However,the widespread application of SMBs as a viable technology remains a great challenge,such as uneven metallic deposition and dendrite formation during cycling.Carbon skeletons as sodiophilic hosts can alleviate the dendrite formation during the plating/stripping.For the carbon skeleton,how to rationalize the design sodiophilic interfaces between the sodium metal and carbon species remains key to developing desirable Na anodes.Herein,we fabricated four kinds of structural features for carbon skeletons using conventional calcination and flash Joule heating.The roles of conductivity,defects,oxygen content,and the distribution of graphite for the deposition of metallic sodium were discussed in detail.Based on interface engineering,the J1600 electrode,which has abundant Na-C species on its surface,showed the highest sodiophilic.There are uniform and rich F-Na species distributed in the inner solid electrolyte interface layer.This study investigated the different Na-deposition behavior in carbon hosts with distinct graphitic arrangements to pave the way for designing and optimizing advanced electrode materials.

Homogenous metallic deposition regulated by abundant lithiophilic sites in nickel/cobalt oxides nanoneedle arrays for lithium metal batteries

Although lithium(Li)metal delivers the highest theoretical capacity as a battery anode,its high reactivity can generate Li dendrites and"dead"Li during cycling,resulting in poor reversibility and low Li utilization.Inducing uniform Li plating/stripping is the core of solving these problems.Herein,we design a highly lithiophilic carbon film with an outer sheath of the nanoneedle arrays to induce homogeneous Li plating/stripping.The excellent conductivity and 3D framework of the carbon film not only offer fast charge transport across the entire electrode but also mitigate the volume change of Li metal during cycling.The abundant lithiophilic sites ensure stable Li plating/stripping,thereby inhibiting the Li dendritic growth and"dead"Li formation.The resulting composite anode allows for stable Li stripping/plating under 0.5 mA cm^(-2) with a capacity of 0.5 mA h cm^(-2) for 4000 h and 3 mA cm^(-2) with a capacity of3 mA h cm^(-2) for 1000 h.The Ex-SEM analysis reveals that lithiophilic property is different at the bottom,top,or channel in the structu re,which can regulate a bottom-up uniform Li deposition behavior.Full cells paired with LFP show a stable capacity of 155 mA h g^(-1) under a current density of 0.5C.The pouch cell can keep powering light-emitting diode even under 180°bending,suggesting its good flexibility and great practical applications.

Lightweight Biobased Polyurethane Nanocomposite Foams Reinforced with Pineapple Leaf Nanofibers (PLNFs)

Pineapple leaf nanofibers(PLNFs)extracted from pineapple leaf fiber were used for reinforcing biobased polyurethane foam(BPU).The dispersion performance of PLNF in the foaming mixture system,nanocomposite foaming behavior,cell morphology,cell size,density,compressive strength and dimensional stability were investigated.The viscosity of the mixtures increased with increasing the PLNF content.The addition of a tiny amount of PLNF did not influence the exothermic temperature of the foam system,but reduced the expansion and gel time of the nanocomposite foams.This reduced time was found to increase the production efficiency.Scanning electron microscopy(SEM)images showed that the PLNF neither affected the cell shape nor size.While the density of the foam was not obviously altered with the addition of a small amount of PLNF,the compressive strength and dimensional stability were significantly improved.

The effect of catalyst layer design on catalyst utilization in PEMFC studied via stochastic reconstruction method

Catalyst utilization is an important determinant of proton exchange membrane fuel cell performance,and increasing the catalyst utilization is one of the most critical approaches to reducing the catalyst loading in PEMFC.4-phase stochastic reconstruction method based on the variable-resolution Quartet Structure Generation Set(QSGS)algorithm is utilized to elucidate the influence of different parameters of electrode preparation,including the porosity,the dispersion degree of carbon agglomerate,ionomer content,and carbon support size,on the catalyst utilization in the catalyst layer.It was found that there exist optimal values for the porosity,dispersion degree of carbon agglomerate,ionomer content,and carbon support sizes in CLs and any deviations from these optimal values would lead to transport issues of electron,proton and mass within CLs.Taking electron,proton and mass transport into consideration simultaneously,the optimal Pt utilization is 46.55%among 48 cases in this investigation,taken at the carbon support diameter of 40 nm,the porosity of 0.4,the agglomerate spatial density of 25μm^(−3) and I/C at 0.7.The selection of porosity,ultrasonic dispersion technique and ionomer content for conventional electrode preparation requires compromises on mass,electron and proton transport,leading to catalyst utilization in CLs hardly exceeding 50%.Therefore,the next generation of catalyst layer design and preparation technology is desired.

低铂质子交换膜燃料电池氧还原催化剂的研究进展与展望

Pt基催化剂是氧还原反应(oxygen reduction reaction,ORR)最有效的催化剂,然而有限的Pt资源和高Pt载量严重制约了质子交换膜燃料电池(proton exchange membrane fuel cells,PEMFCs)的规模化应用.开发同时具有低Pt含量、高活性的ORR催化剂是推动PEMFCs大规模商业化的有效途径.本文从纯Pt催化ORR的机理出发,对当前研究中具有优异性能的均匀Pt合金催化剂和核-壳结构Pt基催化剂的ORR催化机理进行了阐述,并概述了其研究进展、研究策略和制备方法.尽管目前的研究致力于对Pt基纳米颗粒的形貌、粒径、元素组成和晶面等进行精确设计和调控,并在实验室层面实现了活性和耐久性的显著提升,但是现有常用制备方法存在的问题使得其商业化生产无法取得突破进展.最后对Pt基催化剂的规模化制备提出了见解,并对其前景进行了展望.

Hydrogen-assisted scalable preparation of ultrathin Pt shells onto surfactant-free and uniform Pd nanoparticles for highly efficient oxygen reduction reaction in practical fuel cells

Concentrating active Pt atoms in the outer layers of electrocatalysts is a very effective approach to greatly reduce the Pt loading without compromising the electrocatalytic performance and the total electrochemically active surface area(ECSA)for the oxygen reduction reaction(ORR)in hydrogen-based proton-exchange membrane fuel cells.Accordingly,a facile,low-cost,and hydrogen-assisted two-step method is developed in this work,to massively prepare carbon-supported uniform,small-sized,and surfactant-free Pd nanoparticles(NPs)with ultrathin~3-atomic-layer Pt shells(Pd@Pt_(3L) NPs/C).Comprehensive physicochemical characterizations,electrochemical analyses,fuel cell tests,and density functional theory calculations reveal that,benefiting from the ultrathin Pt-shell nanostructure as well as the resulting ligand and geometric effects,Pd@Pt_(3L) NPs/C exhibits not only significantly enhanced ECSA,electrocatalytic activity,and noble-metal(NM)utilization compared to commercial Pt/C,showing 81.24 m^(2)/gPt,0.710 mA/cm^(2),and 352/577 mA/mgNM/Pt in ECSA,area-,and NM-/Pt-mass-specific activity,respectively;but also a much better electrochemical stability during the 10,000-cycle accelerated degradation test.More importantly,the corresponding 25-cm^(2) H2-air/O_(2) fuel cell with the low cathodic Pt loading of~0.152 mgPt/cm^(2)geo achieves the high power density of 0.962/1.261 W/cm^(2)geo at the current density of only 1,600 mA/cm^(2)geo,which is much higher than that for the commercial Pt/C.This work not only develops a high-performance and practical Pt-based ORR electrocatalyst,but also provides a scalable preparation method for fabricating the ultrathin Pt-shell nanostructure,which can be further expanded to other metal shells for other energy-conversion applications.