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1.
Energy Fuels ; 38(12): 11233-11239, 2024 Jun 20.
Artigo em Inglês | MEDLINE | ID: mdl-38919652

RESUMO

Sulfur holds immense promise for battery applications owing to its abundant availability, low cost, and high capacity. Currently, sulfur is commonly combined with alkali or alkaline earth metals in metal-sulfur batteries. However, these batteries universally face challenges in cycling stability due to the inevitable issue of polysulfide dissolution and shuttling. Additionally, the inferior stability of metal sulfide discharge compounds results in low S0/S2- redox potentials (<-0.41 V vs SHE). Herein, we leverage the principle of the hard-soft acid-base theory to introduce a novel silver-sulfur (Ag-S) battery system, which operates on the reaction between the soft acid of Ag+ and the soft base of S2-. Due to their high reaction affinity, the discharge compound of silver sulfide (Ag2S) is intrinsically insoluble and fundamentally stable. This not only resolves the polysulfide dissolution issue but also leads to a predominantly high S0/S2- redox potential (+1.0 V vs. SHE). We thus exploit the Ag-S reaction for a primary zinc battery application, which exhibits a high capacity of ∼620 mAh g-1 and a high voltage of ∼1.45 V. This work offers valuable insights into the application of classic chemistry theories in the development of innovative energy storage devices.

2.
J Neurosurg Spine ; : 1-11, 2024 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-38905708

RESUMO

OBJECTIVE: Cervical spondylotic myelopathy (CSM) stands as the most prevalent form of spinal cord injury, frequently prompting various changes in both the brain and spinal cord. However, the precise nature of these changes within the brains and spinal cords of CSM patients experiencing hand clumsiness (HCL) symptoms has remained elusive. The authors aimed to scrutinize these alterations and explore potential links between these changes and the onset of HCL symptoms. METHODS: Using the modified Japanese Orthopaedic Association (mJOA) scale, the authors classified CSM patients into two groups: those without HCL and those with HCL. The authors performed voxel-wise z-score transformation amplitude of low-frequency fluctuations (zALFF) and resting-state functional connectivity (FC) evaluations in the brain. Additionally, they used the Spinal Cord Toolbox to calculate the fractional anisotropy (FA) of spinal cord tracts. The analysis also encompassed an examination of the correlation of these measures with improvements in mJOA scores. RESULTS: Significant disparities in zALFF values surfaced in the right calcarine, right cuneus, right precuneus, right middle occipital gyrus (MOG), right superior occipital gyrus (SOG), and right superior parietal gyrus (SPG) between healthy controls (HC), patients without HCL, and patients with HCL, primarily within the visual cortex. In the patient group, patients with HCL displayed reduced FC between the right calcarine, right MOG, right SOG, right SPG, right SFG, bilateral MFG, and left median cingulate and paracingulate gyri when compared with patients without HCL. Moreover, significant differences in FA values of the corticospinal tract (CST) and reticulospinal tract (REST) at the C2 level emerged among HC, patients without HCL, and patients with HCL. Notably, zALFF, FC, and FA values in specific brain regions and spinal cord tracts exhibited correlations with mJOA upper-extremity scores. Additionally, FA values of the CST and REST correlated with zALFF values in the right calcarine, right MOG, right SOG, and right SPG. CONCLUSIONS: Alterations within brain regions associated with the visual cortex, the fronto-parietal-occipital attention network, and spinal cord pathways appear to play a substantial role in the emergence and progression of HCL symptoms. Furthermore, the existence of a potential connection between the spinal cord and the brain suggests that this link might be related to the clinical symptoms of CSM.

3.
Neurosurg Focus ; 56(6): E10, 2024 06.
Artigo em Inglês | MEDLINE | ID: mdl-38823056

RESUMO

OBJECTIVE: Hoffmann's sign testing is a commonly used physical examination in clinical practice for patients with cervical spondylotic myelopathy (CSM). However, the pathophysiological mechanisms underlying its occurrence and development have not been thoroughly investigated. Therefore, the present study aimed to explore whether a positive Hoffmann's sign (PHS) in CSM patients is associated with spinal cord and brain remodeling and to identify potential neuroimaging biomarkers with diagnostic value. METHODS: Seventy-six patients with CSM and 40 sex- and age-matched healthy controls (HCs) underwent multimodal MRI. Based on the results of the Hoffmann's sign examination, patients were divided into two groups: those with a PHS (n = 38) and those with a negative Hoffmann's sign (NHS; n = 38). Quantification of spinal cord and brain structural and functional parameters of the participants was performed using various methods, including functional connectivity analysis, voxel-based morphometry, and atlas-based analysis based on functional MRI and structural MRI data. Furthermore, this study conducted a correlation analysis between neuroimaging metrics and neurological function and utilized a support vector machine (SVM) algorithm for the classification of PHS and NHS. RESULTS: In comparison with the NHS and HC groups, PHS patients exhibited significant reductions in the cross-sectional area and fractional anisotropy (FA) of the lateral corticospinal tract (CST), reticulospinal tract (RST), and fasciculus cuneatus, concomitant with bilateral reductions in the volume of the lateral pallidum. The functional connectivity analysis indicated a reduction in functional connectivity between the left lateral pallidum and the right angular gyrus in the PHS group. The correlation analysis indicated a significant positive association between the CST and RST FA and the volume of the left lateral pallidum in PHS patients. Furthermore, all three variables exhibited a positive correlation with the patients' motor function. Finally, using multimodal neuroimaging metrics in conjunction with the SVM algorithm, PHS and NHS were classified with an accuracy rate of 85.53%. CONCLUSIONS: This research revealed a correlation between structural damage to the pallidum and RST and the presence of Hoffmann's sign as well as the motor function in patients with CSM. Features based on neuroimaging indicators have the potential to serve as biomarkers for assessing the extent of neuronal damage in CSM patients.


Assuntos
Imageamento por Ressonância Magnética , Neuroimagem , Doenças da Medula Espinal , Espondilose , Humanos , Masculino , Feminino , Pessoa de Meia-Idade , Espondilose/diagnóstico por imagem , Neuroimagem/métodos , Doenças da Medula Espinal/diagnóstico por imagem , Imageamento por Ressonância Magnética/métodos , Idoso , Adulto , Vértebras Cervicais/diagnóstico por imagem
4.
ACS Appl Energy Mater ; 7(5): 2048-2056, 2024 Mar 11.
Artigo em Inglês | MEDLINE | ID: mdl-38655492

RESUMO

Voltaic pile, the very first battery built by humanity in 1800, plays a seminal role in battery development history. However, the premature design leads to the inevitable copper ion dissolution issue, which dictates its primary battery nature. To address this issue, solid-state electrolytes, ion exchange membranes, and/or sophisticated electrolytes are widely utilized, leading to high costs and complicated cell configuration. Herein, we build a rechargeable zinc-copper voltaic battery from simple and cheap electrolyte/separator materials, thus eliminating the need to use the above components. Notably, our battery leverages the Zn4SO4(OH)6·xH2O precipitation in ZnSO4 electrolytes, a common side reaction in zinc batteries, to provide a "locally alkaline" environment for copper electrodes. Consequently, oxide (O2-) anion insertion takes place and readily transforms copper to copper(I) oxide (Cu2O) without any copper ion dissolution issue. Therefore, this battery realizes a high capacity of ∼370 mA h g-1 and a long cycling of ∼500 cycles. Our work provides an innovative approach to stabilize anion insertion in metal electrodes for energy storage.

5.
Angew Chem Int Ed Engl ; 63(19): e202400110, 2024 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-38484279

RESUMO

The electrolyte concentration not only impacts the battery performance but also affects the battery cost and manufacturing. Currently, most studies focus on high-concentration (>3 M) or localized high-concentration electrolytes (~1 M); however, the expensive lithium salt imposes a major concern. Most recently, ultralow concentration electrolytes (<0.3 M) have emerged as intriguing alternatives for battery applications, which feature low cost, low viscosity, and extreme-temperature operation. However, at such an early development stage, many works are urgently needed to further understand the electrolyte properties. Herein, we introduce an ultralow concentration electrolyte of 2 wt % (0.16 M) lithium difluoro(oxalato)borate (LiDFOB) in standard carbonate solvents. This electrolyte exhibits a record-low salt/solvent mass ratio reported to date, thus pointing to a superior low cost. Furthermore, this electrolyte is highly compatible with commercial Li-ion materials, forming stable and inorganic-rich interphases on the lithium cobalt oxide (LiCoO2) cathode and graphite anode. Consequently, the LiCoO2-graphite full cell demonstrates excellent cycling performance. Besides, this electrolyte is moisture-resistant and effectively suppresses the generation of hydrogen fluoride, which will markedly facilitate the battery assembly and recycling process under ambient conditions.

6.
Neuroimage ; 290: 120558, 2024 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-38437909

RESUMO

The prolonged duration of chronic low back pain (cLBP) inevitably leads to changes in the cognitive, attentional, sensory and emotional processing brain regions. Currently, it remains unclear how these alterations are manifested in the interplay between brain functional and structural networks. This study aimed to predict the Oswestry Disability Index (ODI) in cLBP patients using multimodal brain magnetic resonance imaging (MRI) data and identified the most significant features within the multimodal networks to aid in distinguishing patients from healthy controls (HCs). We constructed dynamic functional connectivity (dFC) and structural connectivity (SC) networks for all participants (n = 112) and employed the Connectome-based Predictive Modeling (CPM) approach to predict ODI scores, utilizing various feature selection thresholds to identify the most significant network change features in dFC and SC outcomes. Subsequently, we utilized these significant features for optimal classifier selection and the integration of multimodal features. The results revealed enhanced connectivity among the frontoparietal network (FPN), somatomotor network (SMN) and thalamus in cLBP patients compared to HCs. The thalamus transmits pain-related sensations and emotions to the cortical areas through the dorsolateral prefrontal cortex (dlPFC) and primary somatosensory cortex (SI), leading to alterations in whole-brain network functionality and structure. Regarding the model selection for the classifier, we found that Support Vector Machine (SVM) best fit these significant network features. The combined model based on dFC and SC features significantly improved classification performance between cLBP patients and HCs (AUC=0.9772). Finally, the results from an external validation set support our hypotheses and provide insights into the potential applicability of the model in real-world scenarios. Our discovery of enhanced connectivity between the thalamus and both the dlPFC (FPN) and SI (SMN) provides a valuable supplement to prior research on cLBP.


Assuntos
Conectoma , Dor Lombar , Humanos , Dor Lombar/diagnóstico por imagem , Encéfalo , Tálamo , Imageamento por Ressonância Magnética/métodos
7.
Brain Res Bull ; 205: 110837, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-38043647

RESUMO

Neuroimaging research has revealed significant changes in brain structure and function in patients with cervical spondylotic myelopathy(CSM). The thalamus plays a crucial role in this process, although its mechanisms of action remain incompletely understood. This study aimed to investigate whether spinal cord compression leads to alterations in the functional connectivity between the thalamus and the cerebral cortex, and to determine if such changes are associated with structural and functional remodeling of the brain in patients with CSM, and to identify potential neuroimaging biomarkers for classification. The study included 40 patients with CSM and 34 healthy controls(HCs) who underwent resting-state functional magnetic resonance imaging(fMRI) and structural MRI scans. Brain structural and functional metrics were quantified using functional connectivity(FC), fractional amplitude of low-frequency fluctuations(fALFF), surface-based morphometry(SBM), and independent component analysis(ICA) based on functional and structural MRI. Patients with CSM exhibited significantly reduced fALFF in the bilateral lateral lingual gyrus, bilateral calcarine fissure, left precentral gyrus and postcentral gyrus, left middle and superior occipital gyrus, left superior marginal gyrus, left inferior parietal gyrus, and right Rolandic operculum. ICA results revealed weakened functional connectivity between the sensorimotor network (SMN) and the left and right frontoparietal network(FPN), and lateral visual network (lVN), along with decreased connectivity between lVN and rFPN, and increased connectivity between lFPN and rFPN. Patients with CSM also had decreased sulcus depth in the bilateral insula, left precentral and postcentral gyrus, and right lingual gyrus and calcarine fissure. Furthermore, cervical spondylotic myelopathy patients showed decreased functional connectivity between the left ventral posterolateral nucleus (VPL) of the thalamus and the right middle occipital gyrus (MOG). Finally,multimodal neuroimaging with support vector machine(SVM) classified patients with CSM and healthy controls with 86.00% accuracy. Our study revealed that the decrease in functional connectivity between the thalamus and cortex mediated by spinal cord compression leads to structural and functional reorganization of the cortex. Features based on neuroimaging markers have the potential to become neuroimaging biomarkers for CSM.


Assuntos
Compressão da Medula Espinal , Doenças da Medula Espinal , Humanos , Córtex Cerebral/diagnóstico por imagem , Imageamento por Ressonância Magnética/métodos , Tálamo/diagnóstico por imagem , Biomarcadores
8.
J Am Chem Soc ; 2023 Nov 07.
Artigo em Inglês | MEDLINE | ID: mdl-37933870

RESUMO

Aqueous batteries using multivalent metals hold great promise for energy storage due to their low cost, high energy, and high safety. Presently, divalent metals (zinc, iron, nickel, and manganese) prevail as the leading choice, which, however, suffer from low Coulombic efficiency or dendrite growth. In stark contrast, trivalent metals have received rare attention despite their capability to unlock unique redox reactions. Herein, we investigate trivalent indium as an innovative and high-performance metal anode for aqueous batteries. The three-electron In3+/In redox endows a high capacity of ∼700 mAh g-1, on par with the Zn metal. Besides, indium exhibits a suitable redox potential (-0.34 V vs standard hydrogen electrode) and dendrite-free plating process, which renders an ultrahigh Coulombic efficiency of 99.3-99.8%. More surprisingly, it features an exceedingly low polarization of 1 mV in symmetrical cells, which is 1-2 orders of magnitude lower than any reported metals. The In-MnO2 full cell also delivers impressive performance, with a cell voltage of ∼1.2 V, a high capacity of ∼330 mAh g-1, and a long cycling time of 680 cycles. Our work exemplifies the efficacy of exploiting trivalent metals as an excellent metal anode, which provides an exciting direction for building high-performance aqueous batteries.

9.
ACS Appl Mater Interfaces ; 15(21): 25536-25549, 2023 May 31.
Artigo em Inglês | MEDLINE | ID: mdl-37200497

RESUMO

Lithium-ion batteries (LIBs) have been widely used for portable electronics and electric vehicles; however, the low capacity in the graphite anode limits the improvement of energy density. Transition-metal selenides are promising anode material candidates due to their high theoretical capacity and controllable structure. In this study, we successfully synthesize a bimetallic transition-metal selenide nanocube composite, which is well embedded in a nitrogen-doped carbon matrix (denoted as CoNiSe2/NC). This material shows a high capacity and excellent cycling for Li-ion storage. Specifically, the reversible capacity approaches ∼1245 mA h g-1 at 0.1 A g-1. When cycled at 1 A g-1, the capacity still remains at 642.9 mA h g-1 even after 1000 cycles. In-operando XRD tests have been carried out to investigate the lithium storage mechanism. We discover that the outstanding performance is due to the unique CoNiSe2/NC nanocomposite characteristics, such as the synergistic effect of bimetallic selenide on lithium storage, the small particle size, and the stable and conductive carbon structure. Therefore, this morphology structure not only reduces the volume change of metal selenides but also produces more lithium storage active sites and shortens lithium diffusion paths, which results in high capacity, good rate, and long cycling.

10.
Front Neurosci ; 17: 1087945, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-36816111

RESUMO

Introduction: Cervical spondylotic myelopathy (CSM) is a common form of non-traumatic spinal cord injury (SCI) and usually leads to remodeling of the brain and spinal cord. In CSM with gait instability, the remodeling of the brain and cervical spinal cord is unclear. We attempted to explore the remodeling of these patients' brains and spinal cords, as well as the relationship between the remodeling of the brain and spinal cord and gait instability. Methods: According to the CSM patients' gait, we divided patients into two groups: normal gait patients (nPT) and abnormal gait patients (aPT). Voxel-wise z-score transformation amplitude of low-frequency fluctuations (zALFF) and resting-state functional connectivity (rs-FC) were performed for estimating brain changes. Cross-sectional area (CSA) and fractional anisotropy (FA) of the spinal cord were computed by Spinal cord toolbox. Correlations of these measures and the modified Japanese Orthopedic Association (mJOA) score were analyzed. Results: We found that the zALFF of caudate nucleus in aPT was higher than that in healthy controls (HC) and lower than that in nPT. The zALFF of the right postcentral gyrus and paracentral lobule in HC was higher than those of aPT and nPT. Compared with the nPT, the aPT showed increased functional connectivity between the caudate nucleus and left angular gyrus, bilateral precuneus and bilateral posterior cingulate cortex (PCC), which constitute a vital section of the default mode network (DMN). No significantly different FA values or CSA of spinal tracts at the C2 level were observed between the HC, nPT and aPT groups. In CSM, the right paracentral lobule's zALFF was negatively correlated with the FA value of fasciculus gracilis (FCG), and the right caudate zALFF was positively correlated with the FA value of the fasciculus cuneatus (FCC). The results showed that the functional connectivity between the right caudate nucleus and DMN was negatively correlated with the CSA of the lateral corticospinal tract (CST). Discussion: The activation of the caudate nucleus and the strengthening functional connectivity between the caudate nucleus and DMN were associated with gait instability in CSM patients. Correlations between spinal cord and brain function might be related to the clinical symptoms in CSM.

11.
Front Aging Neurosci ; 14: 784263, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-35444527

RESUMO

Degenerative cervical myelopathy is a progressive neurodegenerative disease, that has become increasingly prevalent in the aging population worldwide. The current study determined the factors affecting degeneration in the sensorimotor tract with degenerative cervical myelopathy and its relationship with brain structure. We divided patients into hyperintensity (HS) and non-hyperintensity (nHS) groups and measured the fractional anisotropy and apparent diffusion coefficients of the lateral corticospinal tract (CST), fasciculus gracilis and fasciculus cuneatus (FGC). Voxel-based morphometry (VBM) and tract-based spatial statistics (TBSS) techniques were used to estimate brain structure changes. Correlation of the modified Japanese Orthopaedic Association (mJOA) score, light touch, pinprick, motor score, and fractional anisotropy (FA) ratios of the CST at different levels were analyzed. Compared to healthy controls, the FA ratios of CST in the HS and nHS groups were decreased at all levels, and the apparent diffusion coefficient (ADC) ratio was increased only at C4/5 levels in the HS group. The FA ratio of FGC was decreased at the C3/4 and C4/5 levels in the HS group and only decreased at the C4/5 level in the nHS group. The ADC ratio was decreased only at the C4/5 level in the HS group. VBM analysis revealed that the volume of the precentral gyrus, postcentral gyrus, and paracentral lobule increased in patients compared to controls. TBSS analysis found no statistical significance between the sensory and motor tracts in white matter. The volume of clusters in HS and nHS groups negatively correlated with the C1/2 FA ratio of the CST. The results showed that the degeneration distance of the CST was longer than the FGC, and the degeneration distance was related to the degree of compression and spinal cord damage. Structural compensation and the neurotrophin family may lead to enlargement of the brain.

12.
Anal Sci ; 38(4): 675-682, 2022 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-35286648

RESUMO

African swine fever virus (ASFV) causes hemorrhagic infectious disease in pigs with a fatality rate of nearly 100%. In this study, we developed a visual strand exchange amplification detection assay for ASFV. In the presence of ASFV, DNA amplification products containing multimeric G-quadruplex sequences were amplified by strand exchange amplification. These G-quadruplexes, assembled with hemin to form DNAzyme, displayed enhanced significant "turned-on" colorimetric signals to indicate detection results. The results showed that dimeric DNAzyme had the best visualization effect. Under the optimal reaction parameters, there was a linear relationship between the absorbance of the reaction solution at 417 nm and the logarithm of ASFV concentration ranged from 1 × 101 to 1 × 103 copies/µL, and the detection limit was 2.7 copies/µL. We hoped this visual assay could be helpful in the rapid and sensitive detection of ASFV, and the results of multimeric G-quadruplex/hemin DNAzyme could be helpful for the development of better visual detection assays.


Assuntos
Vírus da Febre Suína Africana , Técnicas Biossensoriais , DNA Catalítico , Quadruplex G , Vírus da Febre Suína Africana/genética , Vírus da Febre Suína Africana/metabolismo , Animais , Técnicas Biossensoriais/métodos , Colorimetria , DNA Catalítico/metabolismo , Hemina , Suínos
13.
Biosens Bioelectron ; 205: 114097, 2022 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-35219019

RESUMO

Machine learning algorithms as a powerful tool can efficiently utilize and process large quantities of data generated by high-throughput experiments in various fields. In this work, we used a general ionic salt-assisted synthesis method to prepare oxidase-like Fe-N-C SANs. The possible reason for the excellent enzyme-mimicking activity and affinity of Fe-N-C SANs was further verified by density functional theory calculations. Due to the remarkable oxidase-mimicking activity, the prepared Fe-N-C SANs were used to detect ascorbic acid (AA) with a detection limit of 0.5 µM. Based on the machine learning algorithms, we successfully distinguished six antioxidants (ascorbic acid, glutathione, L-cysteine, dithiothreitol, uric acid, and dopamine) with the same concentration by either one kind of Fe-N-C SANs or three kinds of different Fe-N-C SANs. The usefulness of the Fe-N-C SANs sensor arrays was further validated by the hierarchal cluster analysis, where they also can be correctly identified. More importantly, a SANs-based digital-image colorimetric sensor array has also been successfully constructed and thereby achieved visual and informative colorimetric analysis for practical samples out of the lab. This work not only provides a design synthesis method to prepare SANs but also combines machine learning algorithms with SANs sensors to identify analytes with similar properties, which can further expand to the detection of proteins and cells related to diseases in the future.


Assuntos
Antioxidantes , Técnicas Biossensoriais , Ácido Ascórbico , Colorimetria , Glutationa
14.
J Virol Methods ; 301: 114437, 2022 03.
Artigo em Inglês | MEDLINE | ID: mdl-34933045

RESUMO

COVID-19, a new respiratory infectious disease, was first reported at the end of 2019, in Wuhan, China. Now, COVID-19 is still causing major loss of human life and economic productivity in almost all countries around the world. Early detection, early isolation, and early diagnosis of COVID-19 patients and asymptomatic carriers are essential to blocking the spread of the pandemic. This paper briefly reviewed COVID-19 diagnostic assays for clinical application, including nucleic acid tests, immunological methods, and Computed Tomography (CT) imaging. Nucleic acid tests (NAT) target the virus genome and indicates the existence of the SARS-CoV-2 virus. Currently, real-time quantitative PCR (qPCR) is the most widely used NAT and, basically, is the most used diagnostic assay for COVID-19. Besides qPCR, many novel rapid and sensitive NAT assays were also developed. Serological testing (detection of serum antibodies specific to SARS-CoV-2), which belongs to the immunological methods, is also used in the diagnosis of COVID-19. The positive results of serological testing indicate the presence of antibodies specific to SARS-CoV-2 resulting from being infected with the virus. Viral antigen detection assays are also important immunological methods used mainly for rapid virus detection. However, only a few of these assays had been reported. CT imaging is still an important auxiliary diagnosis tool for COVID-19 patients, especially for symptomatic patients in the early stage, whose viral load is low and different to be identified by NAT. These diagnostic techniques are all good in some way and applying a combination of them will greatly improve the accuracy of COVID-19 diagnostics.


Assuntos
COVID-19 , Humanos , Pandemias , Reação em Cadeia da Polimerase em Tempo Real , SARS-CoV-2 , Sensibilidade e Especificidade , Testes Sorológicos/métodos
15.
ACS Mater Au ; 2(1): 63-71, 2022 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-36855695

RESUMO

Aqueous sodium-ion batteries represent a promising approach for stationary energy storage; however, the lack of appropriate anode materials has substantially retarded their development. Herein, we demonstrated an iron-based phosphate material of Na3Fe3(PO4)4 as an inexpensive and efficacious anode alternative. While the Fe3+/Fe2+ redox couple renders a two-Na-insertion reaction with desirable potentials, its unique layered structure further facilitates the Na-insertion kinetics and reversibility. Consequently, this electrode exhibits an appealing Na-insertion performance, with a reversible capacity of ∼83 mAh g-1, suitable anode potential of -0.4 V vs Ag/AgCl, excellent rate capability of 200 C, and outstanding cycling of 6000 cycles. Utilizing operando synchrotron X-ray diffraction and X-ray absorption spectroscopy, we revealed the structural evolution of the Na3Fe3(PO4)4 anode during the two-electron reaction, where the extremely small volume expansion (∼3%) enables its fast-charging and long-cycling capability. Our work suggests new considerations of developing versatile iron phosphate compounds as appealing anode materials for energy storage in aqueous electrolytes.

16.
Adv Mater ; 34(5): e2106876, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34648671

RESUMO

Potassium-ion batteries (KIBs) have attracted wide interest for energy storage because of the abundance of the electrode materials involved; however, their electrochemical performances are far behind what can be achieved from lithium-ion batteries (LIBs) or sodium-ion batteries (SIBs). Herein, key promising electrode and electrolyte materials for potassium-ion batteries are identified, the coupled electrochemical reactions in the cell are investigated, and the compatibility between different materials is demonstrated to play the most important role. K2 Mn[Fe(CN)6 ] cathode can deliver a high capacity of ≈125 mAh g-1 and exceptional cycling stability over 61 000 cycles (≈9 months) if the side reactions from the anode can be prevented. Graphite is a good anode material but is subjected to degradation in traditional carbonate electrolytes. New concentrated electrolytes are developed and evaluated. A stable KIB system is demonstrated by coupling a stable K2 Mn[Fe(CN)6 ] cathode, a prepotassiated graphite anode with a concentrated electrolyte to achieve a high energy density of ≈260 Wh kg-1 (based on the active mass of cathode and anode) and good cycling of over 1000 cycles.

17.
Adv Mater ; 33(49): e2105234, 2021 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-34623704

RESUMO

Iron ion batteries using Fe2+ as a charge carrier have yet to be widely explored, and they lack high-performing Fe2+ hosting cathode materials to couple with the iron metal anode. Here, it is demonstrated that VOPO4 ∙2H2 O can reversibly host Fe2+ with a high specific capacity of 100 mAh g-1 and stable cycling performance, where 68% of the initial capacity is retained over 800 cycles. In sharp contrast, VOPO4 ∙2H2 O's capacity of hosting Zn2+ fades precipitously over tens of cycles. VOPO4 ∙2H2 O stores Fe2+ with a unique mechanism, where upon contacting the electrolyte by the VOPO4 ∙2H2 O electrode, Fe2+ ions from the electrolyte get oxidized to Fe3+ ions that are inserted and trapped in the VOPO4 ∙2H2 O structure in an electroless redox reaction. The trapped Fe3+ ions, thus, bolt the layered structure of VOPO4 ∙2H2 O, which prevents it from dissolution into the electrolyte during (de)insertion of Fe2+ . The findings offer a new strategy to use a redox-active ion charge carrier to stabilize the layered electrode materials.

18.
Chem Commun (Camb) ; 57(77): 9918-9921, 2021 Sep 28.
Artigo em Inglês | MEDLINE | ID: mdl-34498654

RESUMO

We demonstrate a disposable aqueous primary battery chemistry that comprises environmentally benign materials of the sulfur cathode and Zn anode in a 1 M ZnCl2 aqueous electrolyte. The Zn-S battery shows a high energy density of 1083.3 Wh kg-1 for sulphur with a flat discharge voltage plateau around 0.7 V. When operating at a high mass loading of 8.3 mg cm-2 for sulfur in the cathode, the battery exhibits a very high areal capacity of 11.4 mA h cm-2 and areal energy of 7.7 mW h cm-2.

19.
ACS Appl Mater Interfaces ; 13(24): 28261-28269, 2021 Jun 23.
Artigo em Inglês | MEDLINE | ID: mdl-34105352

RESUMO

Due to climate variation and global warming, utilization of renewable energy becomes increasingly imperative. Rechargeable potassium-ion batteries (PIBs) have lately attracted much attention due to their earth-abundance and cost-effectiveness. Because soft carbon materials are cheap, abundant, and safe, extensive feasible research studies have indicated that they could become promising anode materials for PIBs. In spite of gaining achievements, fundamental questions regarding effects of the basic structure unit inside soft carbon on potassium storage potential have not been sufficiently addressed yet. Here, a series of soft carbon pyrolyzed from 900 to 2900 °C were systematically and quantitatively characterized by combining Raman spectroscopy, near-edge X-ray absorption fine structure (NEXAFS) spectroscopy, X-ray pair distribution function analysis, and advanced evaluation of wide-angle X-ray scattering data. All these characterizations reveal structural details of soft carbon with increasing pyrolysis temperature. Our results show that the potassium storage behavior, especially the potential plateau is closely correlated to non-uniformity in interlayer distance and defect concentration in soft carbon, which is further confirmed by reverse Monte Carlo (RMC) modeling and density functional theory calculation. On the basis of these results, optimizing strategies are discussed to design an advanced soft carbon anode. This work provides significant insights into the structure engineering of soft carbon for high-performance rechargeable PIBs.

20.
Angew Chem Int Ed Engl ; 59(49): 22007-22011, 2020 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-32805079

RESUMO

A non-aqueous proton electrolyte is devised by dissolving H3 PO4 into acetonitrile. The electrolyte exhibits unique vibrational signatures from stimulated Raman spectroscopy. Such an electrolyte exhibits unique characteristics compared to aqueous acidic electrolytes: 1) higher (de)protonation potential for a lower desolvation energy of protons, 2) better cycling stability by dissolution suppression, and 3) higher Coulombic efficiency owing to the lack of oxygen evolution reaction. Two non-aqueous proton full cells exhibit better cycling stability, higher Coulombic efficiency, and less self-discharge compared to the aqueous counterpart.

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