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1.
J Colloid Interface Sci ; 678(Pt B): 599-608, 2024 Sep 07.
Article in English | MEDLINE | ID: mdl-39265332

ABSTRACT

Direct methanol fuel cells rely on the efficiency of their anode/cathode electrocatalysts to facilitate the methanol oxidation reaction and oxygen reduction reaction, respectively. Platinum-based nanocatalysts are at the forefront due to their superior catalytic properties. However, the high-cost, scarcity, and low CO tolerance of platinum pose challenges for the scalable application of DMFCs. Herein, we report novel ultrathin ternary PtNiRu alloy nanowires to improve Pt utilization and CO tolerance. These novel electrocatalysts incorporate the oxophilic metal Ru into ultrathin PtNi nanowires, aiming to enhance the intrinsic activity of platinum while leveraging the long-term durability and high utilization efficiency provided by the bimetallic synergistic effect. The PtNiRu NWs significantly enhance both mass activity and specific activity for ORR, performing about 6.9 times and 3.9 times better than commercial Pt/C, respectively. After a rigorous durability test of 10,000 cycles, the PtNiRu NWs only exhibited a 25.2 % loss in mass activity. Additionally, for MOR, the MA and SA of PtNiRu NWs exceed that of Pt/C catalyst by 4.30 and 2.72 times, respectively, and exhibit exceptional resistance to CO poisoning. Theoretical insights from density functional theory calculations suggest that the introduction of Ru modulates the d-band center of the surface Pt atoms, which contributes to decreased binding strength of oxygenated species and an elevated dissolution potential, substantiating the enhanced performance metrics, and the durability enhancement stems from the stronger PtM bonds than those in PtNiRu NWs resulted from PtRu covalent interactions. These findings not only provide a new perspective on platinum-based nanocatalysts but also significantly advance the quest for more efficient and durable electrocatalysts for DMFCs, representing a substantial stride in fuel cell technology.

2.
J Appl Stat ; 51(12): 2298-2325, 2024.
Article in English | MEDLINE | ID: mdl-39267707

ABSTRACT

This paper investigates the problem of monitoring the ratio involving three variables, jointly distributed as trivariate normal. The Shewhart-type and two exponentially weighted moving average (EWMA) type schemes for monitoring depth ratio are proposed. The ratio of a normal variable to the average of two other normal variables has wide applications in natural science, production, and engineering. It is defined with slightly different terminology in various contexts, such as depth or aspect ratios. In modern bearing manufacturing, the aspect ratio of width to the average of inner and outer diameters can be an essential indicator of product quality and process stability. While there are many helpful existing charts for monitoring the three components separately or jointly when these characteristics follow a normal distribution, the ratio aspect is often ignored. The Shewhart-type schemes' exact and approximated control limits are considered and analyzed. Numerical results based on Monte-Carlo are conducted using the average run length as a metric with different values of in-control ratio and correlation between the three variables. An application based on the parts manufacturing data illustrates the implementation design of the two control charts. The real-life data analysis shows the efficacy of the proposed monitoring schemes in practice.

3.
J Colloid Interface Sci ; 676: 884-895, 2024 Dec 15.
Article in English | MEDLINE | ID: mdl-39067223

ABSTRACT

Developing high active and stable cost-effective bifunctional electrocatalysts for overall water splitting to produce hydrogen is of vital significance in clean and sustainable energy development. This work has prepared a novel porous unreported MOF (Ni-DPT) as a precursor to successfully synthesize a non-noble bifunctional NiCoP/Ni12P5@NF electrocatalyst through doping strategy and interface engineering. This catalyst is constructed by layered self-supporting arrays with heterojunction interface and rich nitrogen-phosphorus doping. Structural characterizations and the density function theory (DFT) calculations confirm that the interface effect of NiCoP/Ni12P5 heterojunction can regulate the electronic structure of the catalyst to optimize the Gibbs free energy of hydrogen (ΔGH*); simultaneously, the defect-rich layered nanoarrays can expose more active sites, shorten mass transfer distance, and generate a self-supporting structure for in-situ reinforcing the structural stability. As a result, this NiCoP/Ni12P5@NF catalyst exhibits favorable electrocatalytic performance, which simply needs overpotentials of 100 mV for HER and 310 mV for OER, respectively, at a current density of 10 mA·cm-2. The anion exchange membrane electrolyzer assembled with this NiCoP/Ni12P5@NF as both anode and cathode catalysts can operate stably for 200 h at a current density of 100 mA·cm-2 with an insignificant voltage decrease. This work may provide some inspiration for the further rational design of inexpensive non-noble multifunctional electrocatalysts and electrode materials for water splitting to generate hydrogen.

4.
J Colloid Interface Sci ; 675: 1-13, 2024 Dec.
Article in English | MEDLINE | ID: mdl-38964120

ABSTRACT

Birnessite-type MnO2 (δ-MnO2) exhibits great potential as a cathode material for aqueous zinc-ion batteries (AZIBs). However, the structural instability and sluggish reaction kinetics restrict its further application. Herein, a unique protons intercalation strategy was utilized to simultaneously modify the interlayer environment and transition metal layers of δ-MnO2. The intercalated protons directly form strong O  H bonds with the adjacent oxygens, while the increased H2O molecules also establish a hydrogen bond network (O  H···O) between H2O molecules or bond with adjacent oxygens. Based on the Grotthuss mechanism, these bondings ultimately enhance the stability of layered structures and facilitate the rapid diffusion of protons. Moreover, the introduction of protons induces numerous oxygen vacancies, reduces steric hindrance, and accelerates ion transport kinetics. Consequently, the protons intercalated δ-MnO2 (H-MnO2-x) demonstrates exceptional specific capacity of 401.7 mAh/g at 0.1 A/g and a fast-charging performance over 1000 cycles. Density functional theory analysis confirms the improved electronic conductivity and reduced diffusion energy barrier. Most importantly, electrochemical quartz crystal microbalance tests combining with ex-situ characterizations verify the inhibitory effect of the interlayer proton environment on basic zinc sulfate formation. Protons intercalation behavior provides a promising avenue for the development of MnO2 as well as other cathodes in AZIBs.

5.
J Colloid Interface Sci ; 675: 226-235, 2024 Dec.
Article in English | MEDLINE | ID: mdl-38968639

ABSTRACT

Although Li metal is considered the most potential anode for Li based batteries, the repeatedly large volume variation and low Coulombic efficiency (CE) are still serious challenges for commercial application. Herein, the interconnect closed hollow graphene spheres with electronic-ionic bi-functional conduction network containing Li4.4Sn nanoparticles loaded internally and ß-Li3PS4 solid electrolyte layer coated externally (ß-LPS/SG/Li4.4Sn) is proposed to achieve uniform and dense Li deposition. Density functional theory (DFT) calculation and experimental results show that Li4.4Sn owns larger Li binding energy and lower nucleation overpotential than spherical graphene (SG), thus being able to guide Li traversing and depositing inside the hollow spheres. The Tafel curves, Li+ diffusion activation energy and experimental results reveal that the ß-Li3PS4 coating layer significantly improves the ionic conductivity of the negative skeleton, covers the defect sites on the SG surface, provides continuous ion transmission channels and accelerates Li+ migration rate. The synergy of both can inhibit the formation of dendritic Li and reduce side reaction between freshly deposited lithium and the organic electrolyte. It's found that Li is preferentially deposited within the SG, evenly deposited on the spherical shell surface until it's completely filled to obtain a dense lithium layer without tip effect. As a result, the ß-LPS/SG/Li4.4Sn anode exhibits a long life of up to 2800 h, an extremely low overpotential (∼13 mV) and a high CE of 99.8 % after 470 cycles. The LiFePO4-based full cell runs stably with a high capacity retention of 86.93 % after 800 cycles at 1C. It is considered that the novel structure design of Li anode skeleton with electron-ionic bi-functional conduction is a promising direction to construct long-term stable lithium metal anodes.

6.
ACS Appl Mater Interfaces ; 16(24): 31341-31347, 2024 Jun 19.
Article in English | MEDLINE | ID: mdl-38853459

ABSTRACT

Sulfide-based solid electrolytes with high ionic conductivity have attracted a lot of attention. However, the incompatibility and interfacial instability of sulfides with the lithium metal anode have emerged as pivotal constraints on their development. To address this challenge, we proposed and successfully synthesized the BH4- doped argyrodite-type electrolyte Li6PS5Cl0.9(BH4)0.1 by mechanical ball milling and annealing. This electrolyte not only exhibits an exceptionally high ionic conductivity of 2.83 × 10-3 S cm-1 at 25 °C but also demonstrates outstanding electrochemical stability. The Li/Li6PS5Cl0.9(BH4)0.1/Li symmetric cell can stably run for more than 400 h at a current density of 0.2 mA cm-2. In sharp contrast, although the F- doped sample, Li6PS5Cl0.3F0.7, can highly improve Li6PS5Cl's electrochemical stability, the ionic conductivity will reduce dramatically to 6.63 × 10-4 S cm-1. The stepwise current method reveals a critical current density of 3.5 mA cm-2 for Li6PS5Cl0.9(BH4)0.1, which makes it a competitive sulfide-based solid electrolyte. This research offers valuable insights for designing new borohydride-containing solid electrolytes.

7.
Small ; : e2404470, 2024 Jun 27.
Article in English | MEDLINE | ID: mdl-38934337

ABSTRACT

The uncontrollable growth of lithium dendrites and the flammability of electrolytes are the direct impediments to the commercial application of high-energy-density lithium metal batteries (LMBs). Herein, this study presents a novel approach that combines microencapsulation and electrospinning technologies to develop a multifunctional composite separator (P@AS) for improving the electrochemical performance and safety performance of LMBs. The P@AS separator forms a dense charcoal layer through the condensed-phase flame retardant mechanism causing the internal separator to suffocate from lack of oxygen. Furthermore, it incorporates a triple strategy promoting the uniform flow of lithium ions, facilitating the formation of a highly ion-conducting solid electrolyte interface (SEI), and encouraging flattened lithium deposition with active SiO2 seed points, considerably suppressing lithium dendrites growth. The high Coulombic efficiency of 95.27% is achieved in Li-Cu cells with additive-free carbonate electrolyte. Additionally, stable cycling performance is also maintained with a capacity retention rate of 93.56% after 300 cycles in LFP//Li cells. Importantly, utilizing P@AS separator delays the ignition of pouch batteries under continuous external heating by 138 s, causing a remarkable reduction in peak heat release rate and total heat release by 23.85% and 27.61%, respectively, substantially improving the fire safety of LMBs.

8.
J Colloid Interface Sci ; 672: 287-298, 2024 Oct 15.
Article in English | MEDLINE | ID: mdl-38843681

ABSTRACT

Compared with lithium-ion batteries (LIBs), lithium-sulfur batteries (LSBs), based on electrochemical reactions involving multi-step 16-electron transformations provide higher specific capacity (1672 mAh g-1) and specific energy (2600 Wh kg-1), exhibiting great potential in the field of energy storage. However, the inherent insulation of sulfur, slow electrochemical reaction kinetics and detrimental shuttle-effect of lithium polysulfides (LiPSs) restrict the development of LSBs in practical applications. Herein, the iodine-doped carbon nanotubes (I-CNTs) is firstly reported as sulfur host material to the enhance the adsorption-conversion kinetics of LSBs. Iodine doping can significantly improve the polarity of I-CNTs. Iodine atoms with lone pair electrons (Lewis base) in iodine-doped CNTs can interact with lithium cations (Lewis acidic) in LiPSs, thereby anchoring polysulfides and suppressing subsequent shuttling behavior. Moreover, the charge transfer between iodine species (electron acceptor) and CNTs (electron donor) decreases the gap band and subsequently improves the conductivity of I-CNTs. The enhanced adsorption effect and conductivity are beneficial for accelerating reaction kinetics and enhancing electrocatalytic activity. The in-situ Raman spectroscopy, quasi in-situ electrochemical impedance spectroscopy (EIS) and Li2S potentiostatic deposition current-time (i-t) curves were conducted to verify mechanism of complex sulfur reduction reaction (SRR). Owing to above advantages, the I-CNTs@S composite cathode exhibits an ultrahigh initial capacity of 1326 mAh g-1 as well as outstanding cyclicability and rate performance. Our research results provide inspirations for the design of multifunctional host material for sulfur/carbon composite cathodes in LSBs.

9.
Chem Asian J ; 19(17): e202400099, 2024 Sep 02.
Article in English | MEDLINE | ID: mdl-38860661

ABSTRACT

Lithium-sulfur batteries (LSBs) are considered next-generation energy storage and conversion solutions owing to their high theoretical specific capacity and the high abundance/low-cost of sulfur-based cathode materials. However, LSBs still encounter significant challenges, including the low conductivities of sulfur-based materials, severe volumetric expansion of sulfur during the discharge process, and the persistent "shuttle effect" of polysulfides. In recent years, a tremendous amount of research has been conducted to address the above challenges by developing coating and compositing materials and corresponding fabrication strategies for sulfur-based cathode materials. In this study, the surface coating, compositing materials, and fabrication methodologies of LSB cathodes are comprehensively reviewed in terms of advanced materials, structure/component characterization, functional mechanisms, and performance validation. Some technical challenges are analyzed in detail, and possible future research directions are proposed to overcome the challenges toward practical applications of lithium-sulfur batteries.

10.
J Colloid Interface Sci ; 669: 466-476, 2024 Sep.
Article in English | MEDLINE | ID: mdl-38723535

ABSTRACT

Heterostructure engineering is considered a crucial strategy to modulate the intrinsic charge transfer behavior of materials, enhance catalytic activity, and optimize sulfur electrochemical processes. However, parsing the role of heterogeneous interface-structure-property relationships in heterostructures is still a key scientific issue to realize the efficient catalytic conversion of polysulfides. Based on this, molybdenum carbide (Mo2C) was successfully partial reduced to molybdenum metal (Mo) via a thermal reduction at high-temperature and the typical Mo-Mo2C-based Mott-Schottky heterostructures were simultaneously constructed, which realized the modulation of the electronic structure of Mo2C and optimized the conversion process of lithium polysulfides (LPS). Compared with single molybdenum carbide, the modulated molybdenum carbide acts as an electron donor with stronger Mo-S bonding strength as well as higher polysulfide adsorption energy, faster Li2S conversion kinetics, and greatly facilitates the adsorption → catalysis process of LPS. As a result, yolk-shell Mo-Mo2C heterostructure (C@Mo-Mo2C) exhibits excellent cycling performance as a sulfur host, with a discharge specific capacity of 488.41 mAh g-1 for C@Mo-Mo2C/S at 4 C and present an excellent high-rate cyclic performance accompanied by capacity decay rate of 0.08 % per cycle after 400 cycles at 2 C. Heterostructure-acting Mo2C electron distribution modulation engineering may contributes to the understanding of the structure-interface-property interaction law in heterostructures and further enables the efficient modulation of the chemical behavior of sulfur.

11.
Anal Chem ; 96(21): 8221-8233, 2024 05 28.
Article in English | MEDLINE | ID: mdl-38740384

ABSTRACT

Compared with traditional "lock-key mode" biosensors, a sensor array consists of a series of sensing elements based on intermolecular interactions (typically hydrogen bonds, van der Waals forces, and electrostatic interactions). At the same time, sensor arrays also have the advantages of fast response, high sensitivity, low energy consumption, low cost, rich output signals, and imageability, which have attracted widespread attention from researchers. Nanozymes are nanomaterials which own enzyme-like properties. Because of the adjustable activity, high stability, and cost effectiveness of nanozymes, they are potential candidates for construction of sensor arrays to output different signals from analytes through the chemoresponse of colorants, which solves the shortcomings of traditional sensors that they cannot support multiple detection and lack universality. Recently, a sensor array based on nanozymes as nonspecific recognition receptors has attracted much more attention from researchers and has been applied to precise recognition of proteins, bacteria, and heavy metals. In this perspective, attention is given to nanozymes and the regulation of their enzyme-like activity. Particularly, the building principles and methods for sensor arrays based on nanozymes are analyzed, and the applications are summarized. Finally, the approaches to overcome the challenges and perspectives are also presented and analyzed for facilitating further research and development of nanozyme sensor arrays. This perspective should be helpful for gaining insight into research ideas within the field of nanozyme sensor arrays.


Subject(s)
Biosensing Techniques , Nanostructures , Nanostructures/chemistry , Enzymes/metabolism , Enzymes/chemistry
12.
Adv Mater ; 36(32): e2314120, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38578406

ABSTRACT

Solid polymer electrolytes (SPEs) for lithium metal batteries have garnered considerable interests owing to their low cost, flexibility, lightweight, and favorable interfacial compatibility with battery electrodes. Their soft mechanical nature compared to solid inorganic electrolytes give them a large advantage to be used in low pressure solid-state lithium metal batteries, which can avoid the cost and weight of the pressure cages. However, the application of SPEs is hindered by their relatively low ionic conductivity. In addressing this limitation, enormous efforts are devoted to the experimental investigation and theoretical calculations/simulation of new polymer classes. Recently, metal-organic frameworks (MOFs) have been shown to be effective in enhancing ion transport in SPEs. However, the mechanisms in enhancing Li+ conductivity have rarely been systematically and comprehensively analyzed. Therefore, this review provides an in-depth summary of the mechanisms of MOF-enhanced Li+ transport in MOF-based solid polymer electrolytes (MSPEs) in terms of polymer, MOF, MOF/polymer interface, and solid electrolyte interface aspects, respectively. Moreover, the understanding of Li+ conduction mechanisms through employing advanced characterization tools, theoretical calculations, and simulations are also reviewed in this review. Finally, the main challenges in developing MSPEs are deeply analyzed and the corresponding future research directions are also proposed.

13.
J Colloid Interface Sci ; 666: 403-415, 2024 Jul 15.
Article in English | MEDLINE | ID: mdl-38603882

ABSTRACT

Transition metal phosphides have been demonstrated to be promising non-noble catalysts for water splitting, yet their electrocatalytic performance is impeded by unfavorable free energies of adsorbed intermediates. The achievement of nanoscale modulation in morphology and electronic states is imperative for enhancing their intrinsic electrocatalytic activity. Herein, we propose a strategy to expedite the water splitting process over NiCoP/FeNiCoP hollow ellipsoids by modulating the electronic structure and d-band center. These unique phosphorus (P) vacancies-rich ellipsoids are synthesized through an ion-exchange reaction between uniform NiCo-nanoprisms and K3[Fe(CN)6], followed by NaH2PO2-assisted phosphorization under N2 atmosphere. Various characterizations reveals that the titled catalyst possesses high specific surface area, abundant porosity, and accessible inner surfaces, all of which are beneficial for efficient mass transfer and gas diffusion. Moreover, density functional theory (DFT) calculations further confirms that the NiCoP/FeNiCoP heterojunction associated with P vacancies regulate the electronic structures of d-electrons and p-electrons of Co and P atoms, respectively, resulting in a higher desorption efficiency of adsorbed H* intermediates with a lower energy barrier for water splitting. Due to the aforementioned advantages, the resultant NiCoP/FeNiCoP hollow ellipsoids exhibit remarkably low overpotentials of 45 and 266 mV for hydrogen and oxygen evolution reaction to achieve the current densities of 10 and 50 mA cm-2, respectively. This work not only reports the synthesis of a hollow double-shell structure of NiCoP/FeNiCoP but also introduces a novel strategy for constructing a multifunctional electrocatalyst for water splitting.

14.
J Colloid Interface Sci ; 666: 472-480, 2024 Jul 15.
Article in English | MEDLINE | ID: mdl-38613970

ABSTRACT

All-solid-state lithium batteries (ASSLBs) are considered promising energy storage systems due to their high energy density and inherent safety. However, scalable fabrication of ASSLBs based on transition metal sulfide cathodes through the conventional powder cold-pressing method with ultrahigh stacking pressure remains challenging. This article elucidates a dry process methodology for preparing flexible and high-performance FeS2-based ASSLBs under low stack pressure by utilizing polytetrafluoroethylene (PTFE) binder. In this design, fibrous PTFE interweaves Li6PS5Cl particles and FeS2 cathode components, forming flexible electrolyte and composite cathode membranes. Beneficial to the robust adhesion, the composite cathode and Li6PS5Cl membranes are tightly compacted under a low stacking pressure of 100 MPa which is a fifth of the conventional pressure. Moreover, the electrode/electrolyte interface can sustain adequate contact throughout electrochemical cycling. As expected, the FeS2-based ASSLBs exhibit outstanding rate performance and cyclic stability, contributing a reversible discharged capacity of 370.7 mAh g-1 at 0.3C after 200 cycles. More importantly, the meticulous dQ/dV analysis reveals that the three-dimensional PTFE binder effectively binds the discharge products with sluggish kinetics (Li2S and Fe) to the ion-electron conductive network in the composite cathode, thereby preventing the electrochemical inactivation of products and enhancing electrochemical performance. Furthermore, FeS2-based pouch-type cells are fabricated, demonstrating the potential of PTFE-based dry-process technology to scale up ASSLBs from laboratory-scale mold cells to factory-scale pouch cells. This feasible dry-processed technology provides valuable insights to advance the practical applications of ASSLBs.

15.
Dalton Trans ; 53(16): 7035-7043, 2024 Apr 23.
Article in English | MEDLINE | ID: mdl-38563460

ABSTRACT

Although lithium-sulfur (Li-S) batteries have attracted strong consideration regarding their fundamental mechanism and energy applications, the inferior cycling performance and low reaction rate caused by the "shuttling effect" and the sluggish reaction kinetics of lithium polysulfides (LiPSs) impede their practical application. In this work, graphitic C3N4 (g-C3N4) assembled with highly-dispersed nitrogen-containing carbon quantum dots (CQDs) is designed as a cooperative catalyst to accelerate the reaction kinetics of LiPS conversion, the precipitation of Li2S during discharging, and insoluble Li2S decomposition during the charging process. Meanwhile, the introduction of CQDs improves the conductivity of the g-C3N4 substrate, showing great significance for the construction of high-performance electrocatalysts. As a result, the as-obtained composite shows efficient adsorption and electrochemical conversion of LiPSs, and the Li-S batteries assembled with CQDs/g-C3N4 exhibit an initial specific capacity of 1300.0 mA h g-1 at the current density of 0.1C and retain 582.3 mA h g-1 after 200 cycles. The electrode with the modified composite displays a greater capacity contribution of Li2S precipitation (175.7 mA h g-1), indicating an enhanced catalytic activity of g-C3N4 decorated by CQDs. The rational design of CQDs/g-C3N4 as a sulfur host could be an effective strategy for developing high performance Li-S batteries.

16.
Small ; 20(31): e2400139, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38497843

ABSTRACT

The oxygen evolution reaction (OER) performance of NiCo LDH electrocatalysts can be improved through fluorine doping. The roles of Ni and Co active sites in such catalysts remain ambiguous and controversial. In addressing the issue, this study draws upon the molecular orbital theory and proposes the active center competitive mechanism between Ni and Co. The doped F-atoms can directly impact the valence state of metal atoms or exert an indirect influence through the dehydrogenation, thereby modulating the active center. As the F-atoms are progressively aggregate, the eg orbitals of Ni and Co transition from e2 g to e1 g, and subsequently to e0 g. The corresponding valence state elevates from +2 to +3, and then to +4, signifying an initial increase followed by a subsequent decrease in the electrocatalytic performance. Furthermore, a series of F-NiCo LDH catalysts are synthesized to verify the eg orbital occupancy analysis, and the catalytic OER overpotentials are 303, 243, 240, and 246 mV at the current density of 10 mA cm-2, respectively, which coincides well with the theoretical prediction. This investigation not only provides novel mechanistic insights into the transition and competition of Ni and Co in F-NiCo LDH catalysts but also establishes a foundation for the design of high-performance catalysts.

17.
Nanomicro Lett ; 16(1): 111, 2024 Feb 06.
Article in English | MEDLINE | ID: mdl-38321305

ABSTRACT

Hydrogen evolution reaction (HER) has become a key factor affecting the cycling stability of aqueous Zn-ion batteries, while the corresponding fundamental issues involving HER are still unclear. Herein, the reaction mechanisms of HER on various crystalline surfaces have been investigated by first-principle calculations based on density functional theory. It is found that the Volmer step is the rate-limiting step of HER on the Zn (002) and (100) surfaces, while, the reaction rates of HER on the Zn (101), (102) and (103) surfaces are determined by the Tafel step. Moreover, the correlation between HER activity and the generalized coordination number ([Formula: see text]) of Zn at the surfaces has been revealed. The relatively weaker HER activity on Zn (002) surface can be attributed to the higher [Formula: see text] of surface Zn atom. The atomically uneven Zn (002) surface shows significantly higher HER activity than the flat Zn (002) surface as the [Formula: see text] of the surface Zn atom is lowered. The [Formula: see text] of surface Zn atom is proposed as a key descriptor of HER activity. Tuning the [Formula: see text] of surface Zn atom would be a vital strategy to inhibit HER on the Zn anode surface based on the presented theoretical studies. Furthermore, this work provides a theoretical basis for the in-depth understanding of HER on the Zn surface.

18.
Dalton Trans ; 53(11): 5301, 2024 Mar 12.
Article in English | MEDLINE | ID: mdl-38420664

ABSTRACT

Correction for 'Zeolitic imidazolate framework-derived composites with SnO2 and ZnO phase components for electrocatalytic carbon dioxide reduction' by Yayu Guan et al., Dalton Trans., 2022, 51, 7274-7283, https://doi.org/10.1039/d2dt00906d.

19.
J Colloid Interface Sci ; 659: 533-541, 2024 Apr.
Article in English | MEDLINE | ID: mdl-38190780

ABSTRACT

Li metal anodes have high specific capacity and low electrode potential, and have always been considered as one of the most promising anode materials. However, the growth of Li dendrites, unstable solid electrolyte interface layer (SEI), severe side reactions at the Li/electrolyte interface, and infinite volume expansion of the Li anode seriously hinder the practical application of solid-state Li metal batteries (LMBs). Herein, we report a polyurethane elastomer (TPU) material with high elasticity and interfacial stability as a solid polymer electrolyte (SPE) for LMBs. The synergistic effects of its designed soft chain forging (PEO) and hard chain segments (IPDI) can enhance Li ion conductivity, elastic modulus and flexibility of the SPE to settle the challenges of the Li metal anodes. Moreover, Li2S, as a solid-state electrolyte additive, is able to effectively inhibit the occurrence of side reactions at the interface between Li metal and SPE, promote the decomposition of N(CF3SO2)2- and in-situ generation of LiF with low Li+ diffusion barrier and excellent electronic insulation, achieving rapid Li ion transport and uniform Li deposition. As a result, stable cycle of up to 1400 h has been achieved for a Li||TPU-Li2S||Li battery at 0.1 mA/cm2 at 50 ℃, accompanied with a stable cycling performance of 350 h at a higher current density of 0.5 mA/cm2. Finally, the LiFePO4||TPU-Li2S||Li full battery exhibits an excellent cycling performance with a capacity retention rate of 80 % after 500 cycles at 1C. This simple and low-cost strategy provides novel design thoughts for practical application of high-performance SPEs in stable and long-life LMBs.

20.
Chemistry ; 30(3): e202303211, 2024 Jan 11.
Article in English | MEDLINE | ID: mdl-37909248

ABSTRACT

Aqueous zinc-ion batteries (AZIBs) have attracted considerable attention. However, due to the uneven distribution of charge density at Zn anode-electrolyte interface, severe dendrites and corrosion are generated during cycling. In this work, a facile and scalable strategy to address the above-mentioned issues has been proposed through regulating the charge density at Zn anode-electrolyte interface. As a proof of concept, amidinothiourea (ATU) with abundant lone-pair electrons is employed as an interfacial charge modifier for Zn anode-electrolyte interface. The uniform and increased interfacial charge distribution on Zn anode-electrolyte interface has been obtained. Moreover, the unique Zn-bond constructed between N atoms and Zn2+ as well as the hydrogen bonds are formed among ATU and Ac- anion/active H2 O, which promote the migration and desolvation behavior of Zn2+ at anode-electrolyte interface. Accordingly, at a trace concentration of 0.01 mg mL-1 ATU, these features endow Zn anode with a long cycling life (more than 800 h), and a high average Columbic efficiency (99.52 %) for Zn||Cu batteries. When pairing with I2 cathode, the improved cycling ability (5000 cycles) with capacity retention of 77.9 % is achieved. The fundamental understanding on the regulation of charge density at anode-electrolyte interface can facilitate the development of AZIBs.

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