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At least 901 records · Page 50

Synthesis of carbon core–shell pore structures and their performance as supercapacitors

High-power supercapacitors require excellent electrolyte mobility within the pore network and high electrical conductivity for maximum capacitance and efficiency. Achieving high power typically requires sacrificing energy densities, as the latter demands a high specific surface area and narrow porosity that impedes ion transport. Here, we present a novel solution for this optimization problem: a nanostructured core–shell carbonaceous material that exhibits a microporous carbon core surrounded by a mesoporous, graphitic shell. The tunable synthesis parameters yielded a structure that features either a sharp or a gradual transition between the core and shell sections. Electrochemical supercapacitor testing using organic electrolyte revealed that these novel core–shell materials outperform carbons with homogeneous pore structures. The hybrid core–shell materials showed a combination of good capacitance retention, typical for the carbon present in the shell and high specific capacitance, typical for the core material. These materials achieved power densities in excess of 40 kW kg -1 at energy densities reaching 27 Wh kg -1 .

25 ENERGY STORAGE↗

Structure-dependent performance of TiO 2 /C as anode material for Na-ion batteries

The performance of energy storage materials is highly dependent on their nanostructures. Herein, hierarchical rod-in-tube TiO 2 with a uniform carbon coating is synthesized as the anode material for sodium-ion batteries by a facile solvothermal method. This unique structure consists of a tunable nanorod core, interstitial hollow spaces, and a functional nanotube shell assembled from two-dimensional nanosheets. By adjusting the types of solvents used and reaction time, the morphologies of TiO 2 /C composites can be tuned to nanoparticles, microrods, rod-in-tube structures, or microtubes. Among these materials, rod-in-tube TiO 2 with a uniform carbon coating shows the highest electronic conductivity, specific surface area (336.4 m 2 g -1 ), and porosity, and these factors lead to the best sodium storage capability. Benefiting from the unique structural features and improved electronic/ionic conductivity, the as-obtained rod-in-tube TiO 2 /C in coin cell tests exhibits a high discharge capacity of 277.5 and 153.9 mAh g -1 at 50 and 5000 mA g -1 , respectively, and almost 100% capacity retention over 14,000 cycles at 5000 mA g -1 . In operando high-energy X-ray diffraction further confirms the stable crystal structure of the rod-in-tube TiO 2 /C during Na + insertion/extraction. Finally, this work highlights that nanostructure design is an effective strategy to achieve advanced energy storage materials.

25 ENERGY STORAGE↗

Sub-5 nm edge-rich 1T'-ReSe 2 as bifunctional materials for hydrogen evolution and sodium-ion storage

The rhenium-based transition metal dichalcogenides (TMDs), as new members in the TMDs family, have raised great interests recently. Due to the anisotropic structure and unique photoelectric properties, they have potential applications for electrochemical energy conversion and storage. In this work, we performed density functional theory (DFT) calculations on pristine 1T'-ReSe 2 toward hydrogen evolution reaction (HER). The results indicated that the Gibbs free energy of the 1T'-ReSe 2 edge site for HER could be as small as 0.01 eV, superior to other reported TMDs. Experimentally, we developed a strategy to fabricate sub-5 nm sized 1T'-ReSe 2 nanoflakes on carbon nanotubes. Such a small size for the nanoflakes brought abundant edge exposure, which boosted the catalytic activity in the HER. Specifically, the 1T'-ReSe 2 nanoflakes needed only 23 and 60 mV overpotentials to achieve –1 and –10 mA cm –2 current densities, along with a low Tafel slope of 37 mV dec –1 and a high exchange current density of 0.3 mA cm –2 . The edge-rich and layered 1T'-ReSe 2 was also explored as an anode for sodium ion battery. The in operando X-ray absorption near edge structure (XANES) technique was applied to investigate the TMD behavior in real-time during the sodiation/desodiation process. Furthermore, the in situ results revealed that the nanosized 1T'-ReSe 2 is electrchemically reversible during discharge/charge cycles. The electrochemical test results demonstrated that 1T'-ReSe 2 could be a promising anode material for alkaline batteries.

25 ENERGY STORAGE↗

Nitrogen-coordinated single iron atom catalysts derived from metal organic frameworks for oxygen reduction reaction

Iron and nitrogen co-doped carbon (Fe-N-C) catalysts hold great promise to replace platinum group metal used for the oxygen reduction reaction (ORR) in low-temperature fuel cells. However, general synthesis routes require tedious acid washing and extensive heat treatment, usually resulting in uncontrollable morphologies and undesirable compounds. In this work, a zeolitic imidazolate framework (ZIF-8) was employed as a self-template for one-pot synthesis of a Fe-N-C catalyst consisting of uniformly dispersed Fe single atoms. Atomically dispersed Fe atoms were well distributed along the edges of the porous carbon matrix. Each of the Fe atoms was coordinated with four N atoms in the plane and two O atoms in the axial direction. The optimized Fe-N-C catalyst showed excellent ORR activities with half-wave potentials of 0.81 and 0.90 V in acidic and alkaline solutions, respectively. The results may be important for the optimization of single-atom-based catalysts for various reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

1T MoS 2 nanosheets with extraordinary sodium storage properties via thermal-driven ion intercalation assisted exfoliation of bulky MoS 2

Metallic phase (1T) MoS 2 has attracted enormous attention as an appealing energy storage material for batteries, supercapacitors, and catalysts. However, a facile fabrication method is lacking and the intensive understanding of its sodium storage mechanism is absent. Herein, ultrathin 1T MoS 2 nanosheets (1-2 layers) are directly fabricated via and are investigated as an anode material for sodium-ion batteries. Interestingly, the as-prepared 1T MoS 2 nanosheets demonstrate a high reversible capacity of 450 mAh g -1 at 50 mA g -1 and outstanding cycling stability with a high capacity retention ratio of 94% after 200 cycles at 1 A g -1 , which is far superior to that of the 2H phase counterpart. Density function theory (DFT) calculations show that, in addition to significantly enhanced electronic conductivity, 1T MoS 2 also possesses much more sodium philicity and faster Na atom mobility in comparison with the 2H phase. More importantly, as revealed by ex-situ Raman, in-situ X-ray diffraction, and DFT calculations, the 1T MoS 2 is more capable of suppressing the dissolution of S species from the material structure compared with the 2H phase, leading to excellent cycling stability. Furthermore, the facile and easily scalable method as well as the deep mechanism analysis will provide a very important reference for the development of high-performance MoS 2 anodes and other SIB electrode materials.

1T MoS2↗

High rate and long cycle life in Li-O 2 batteries with highly efficient catalytic cathode configured with Co 3 O 4 nanoflower

The reaction mechanism of non-aqueous Li-O 2 batteries is based on the deposition and decomposition of Li 2 O 2 . The polarization of Li-O 2 batteries can be rapidly increased by operation under a high rate condition, resulting in the early capacity fade of the cells. Therefore, a well-designed catalyst with a unique structure and excellent catalytic ability is an important way to boost the round-trip performance of Li-O 2 batteries, especially under high current density. In this work, a unique nanoflower structure assembled with Co 3 O 4 nanosheets is synthesized by using 2-methylimidazole (2-MIM) as a structural directing agent. X-ray photoelectron spectroscopy (XPS) and Raman spectra reveal abundant oxygen vacancies on the surface of the Co 3 O 4 nanoflower, which are beneficial for oxygen reduction and evolution reactions and long round-trip lifetime. Density functional theory results demonstrate that Co 3 O 4 catalyst with oxygen vacancies could promote the wetting of Li 2 O 2 on substrate and formation of a Li 2 O 2 nanofilm, thereby boosting the discharge capacity of Li-O 2 batteries. On account of the synergistic effect of abundant oxygen vacancies, the unique structure, and excellent oxygen evolution reaction, Co 3 O 4 nanoflower-based cells could deliver ultralong lifetime of 276 and 248 cycles with a discharge capacity of 1000 mAh g(-1) under charge/discharge current densities of 0.5 A g -1 and 1 A g -1 , respectively. Finally, this study has shed light on a new strategy for catalyst preparation for long lifetime Li-O 2 batteries.

25 ENERGY STORAGE↗

Toward a high-voltage fast-charging pouch cell with TiO 2 cathode coating and enhanced battery safety

Nickel-rich layered lithium transition metal oxides, LiNi x Co y Mn 1-x-y O 2 , are key cathode materials for high-energy lithium-ion batteries owing to their high specific capacity. However, the commercial deployment of nickel-rich oxides has been hampered by their poor thermostability and insufficient cycle life. In this work full batteries with uncoated and TiO 2 -coated LiNi 0.5 Co 0.2 Mn 0.3 O 2 cathodes and graphite anodes are compared in terms of electrochemical performance and safety behavior. The battery using a TiO 2 -coated LiNi 0.5 Co 0.2 Mn 0.3 O 2 cathode exhibited better cyclic performance at high cutoff voltage. Electrochemical impedance spectroscopy analysis indicated that the TiO 2 -coated LiNi 0.5 Co 0.2 Mn 0.3 O 2 cathode gave the battery a more stable charge transfer resistance. Transmission electron microscopy demonstrated that TiO 2 coating reduced accumulation of the cathode electrolyte interface layer on the particle surface. Time-of-flight secondary ion mass spectrometry demonstrated that TiO 2 coating markedly enhanced the interface stability of the cathode particle and protected the particle from serious etching by the electrolyte. Accelerating rate calorimetry revealed that the trigger temperature of thermal runaway for the battery using TiO 2 -coated LiNi 0.5 Co 0.2 Mn 0.3 O 2 as cathode material was 257 °C, which was higher than that of the battery with the uncoated LiNi 0.5 Co 0.2 Mn 0.3 O 2 cathode (251 °C). In situ X-ray diffraction during heating demonstrated that this enhanced safety can be attributed to the suppressed phase evolution of the coated cathode material.

25 ENERGY STORAGE↗

A practical phosphorus-based anode material for high-energy lithium-ion batteries

State-of-the-art lithium-ion batteries cannot satisfy the increasing energy demand worldwide because of the low specific capacity of the graphite anode. Silicon and phosphorus both show much higher specific capacity; however, their practical use is significantly hindered by their large volume changes during charge/discharge. Although significant efforts have been made to improve their cycle life, the initial coulombic efficiencies of the reported Si-based and P-based anodes are still unsatisfactory (<90%). In this study, by using a scalable high-energy ball milling approach, we report a practical hierarchical micro/nanostructured P-based anode material for high-energy lithium-ion batteries, which possesses a high initial coulombic efficiency of 91% and high specific capacity of ~2500 mAh g –1 together with long cycle life and fast charging capability. In situ high-energy X-ray diffraction and in situ single-particle charging/discharging were used to understand its superior lithium storage performance. Moreover, proof-of-concept full-cell lithium-ion batteries using such an anode and a LiNi 0.6 Co 0.2 Mn 0.2 O 2 cathode were assembled to show their practical use. The findings presented here can serve as a good guideline for the future design of high-performance anode materials for lithium-ion batteries.

25 ENERGY STORAGE↗

Durable hybrid electrocatalysts for proton exchange membrane fuel cells

The low durability of carbon-based non-precious metal electrocatalysts hinders their practical applications in proton exchange membrane fuel cells (PEMFCs). In this study, we rationally design a hybrid Pt-Fe-N-C electrocatalyst with unprecedented durability. It consists of abundant Pt and Fe single atoms homogeneously dispersed on the nitrogen-doped carbon support and a small amount of Pt-Fe alloy nanoparticles. A PEMFC with Pt-Fe-N-C as the cathode shows a larger peak power density (0.75 W cm -2 ) than that with Fe-N-C as the cathode (0.50 W cm -2 ). The remarkable durability of Pt-Fe-N-C is reflected from no noticeable drop in the half-wave potential after 70000 potential cycles between 0.6 and 1.0 V in the liquid cell, and 80% current retention after 85 h of potential hold at 0.4 V in the fuel cell. This work demonstrates the feasibility of improving the durability of Fe-N-C material via ultra-low Pt doping and makes non-precious metal electrocatalysts be close to achieving commercial metrics.

25 ENERGY STORAGE↗

A General Strategy for Batch Development of High-Performance and Cost-Effective Sodium Layered Cathodes

High-performance and low-cost transition metal (TM) layered oxides using earth abundant elements are promising cathodes for Na-ion batteries. However, it is challenging to obtain desired materials because the large Na size, different Na occupations and various layer stacking sequences multiply the complication in determining the structure of a given composition and exacerbate uncertainty to the structure-property correlation. In this work, we use the attainment of desired NaxMnyNiZTM1-y-zO2-based cathode materials as an example to demonstrate a general roadmap for batch development of sodium layered cathodes towards practical applications. A synthesis phase diagram of NaxMnyNi1-yO2 was created for pre-screening and rational selection of the platform material of P2/O3-structured Na0.85Mn0.6Ni0.4O2. Cationic potential was leveraged in elemental substitution to further promote the material structural stability and electrochemical performance. Several cost-effective O3 and P2/O3 hybrid cathode materials have been obtained, all of which demonstrate excellent performance. In particular, the Na0.85Mn0.5Ni0.4Ti0.1O2 delivers a high specific capacity of ~130 mAh/g between 2-4 V and 91% retention after 500 cycles. The work discovers multiple materials as high-performance and cost-effective Na-ion battery cathodes and offers critical guidance to the rational design of future layered cathode materials.

Xiao, Biwei↗

In situ microscopy and spectroscopy characterization of microsized Sn anode for sodium-ion batteries

Microsized Sn is a promising anode material for sodium-ion batteries in terms of cost, specific capacity, and volumetric energy density, which however suffers from huge volume changes and rapid cell degradation upon cycling. Despite recent advances via nanostructured electrode design and interface engineering, the correlation between mechanical stability, solid-electrolyte interphase (SEI) and reaction kinetics/reversibility remains controversial and elusive. Here, in this work, by combining in situ scanning electron microcopy and X-ray absorption spectroscopy as well as X-ray photoelectron spectroscopy, we have investigated the underlying electro-chemo-mechanical behavior and their coupling effects during charge/discharge of microsized Sn anode. Our results revealed that microsized Sn is pulverized into nanoparticles with simultaneous formation of numerous voids and pores upon the 1st charge/discharge, while the electrolytes composition plays a critical role on the consequent parasitic reactions and eventually the sodiation/de-sodiation reversibility. In contrast to carbonate-based electrolytes, ether-based electrolytes enabled formation of inorganic species dominated SEI with improved mechanical strength, thus leading to higher specific capacity and improved cycling stability. The present findings are crucial for future development of microsized anode materials for rechargeable batteries with high volumetric energy density.

25 ENERGY STORAGE↗

Diamond detector technology, status and perspectives

Detectors based on Chemical Vapor Deposition (CVD) diamond have been used extensively and successfully in beam conditions/beam loss monitors as the innermost detectors in the highest radiation areas of Large Hadron Collider (LHC) experiments. The startup of the LHC in 2015 brought a new milestone where the first polycrystalline CVD (pCVD) diamond pixel modules were installed in an LHC experiment and successfully began operation. The RD42 collaboration at CERN is leading the effort to develop polycrystalline CVD diamond as a material for tracking detectors operating in extreme radiation environments. The status of the RD42 project with emphasis on recent beam test results is presented.

3D diamond detectors↗

Results on radiation tolerance of diamond detectors

In sight of the luminosity increase of the High Luminosity-LHC (HL-LHC), most experiments at the CERN Large Hadron Collider (LHC) are planning upgrades for their innermost layers in the next 5–10 years. These upgrades will require more radiation tolerant technologies than exist today. Usage of Chemical Vapor Deposition (CVD) diamond as detector material is one of the potentially interesting technologies for the upgrade. CVD diamond has been used extensively in the beam condition monitors of BaBar, Belle, CDF and all LHC experiments. Measurements of the radiation tolerance of the highest quality polycrystalline CVD material for a range of proton energies, pions and neutrons obtained with this material are presented. In addition, new results on the evolution of various semiconductor parameters as a function of the dose rate are described.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Unraveling plant phenotype to genotype associations with daily hyperspectral traits in Populus trichocarpa

Hyperspectral remote sensing is a powerful, high-throughput phenotyping tool that quantifies physiologically and structurally relevant wavelengths across diverse genotypes and over varying temporal scales. In this study, we combined tower-based continuous hyperspectral sensing with genome-wide association studies to analyze 1423 wavebands (400-900 nm) and derivative vegetation indices across 505 genotypes and the genetic architecture of hyperspectral phenotypes over time in Populus trichocarpa Torr. & Gray grown under field conditions. Wavelengths related to chlorophyll and carotenoid absorption spectra exhibited the strongest genetic variation resulting in 98 significant SNP associations. Notably, we found substantial overlap in genetic association between the blue and red spectral regions, indicative of carotenoids and chlorophyll, respectively, and identified more than 10 candidate genes associated with chloroplast function, underpinning photosynthetic activity. Furthermore, fluctuations in associations for vegetative indices, such as the chlorophyll:carotenoid index (CCI), across the growing season reveal a temporally dynamic genetic architecture of physiological traits associated with fall senescence of this temperate tree species. Finally, we also observed correlations (spearman rho = 0.3, p < 1x10 −8 ) between individual wavebands or vegetative indices and growth rate, assessed as the relative change of tree height over the growing season. The growth rate prediction was substantially improved by a regularization multivariate model (spearman rho>0.5, p < 1x10 −16 ), reinforcing the value of hyperspectral measurements for predicting traits linked to tree productivity. These findings highlight the potential of high-throughput, rapid, hyperspectral genome wide association studies GWAS to uncover physiologically meaningful genetic variation and offer promising insights for future acceleration for plant breeding.

09 BIOMASS FUELS↗