arXiv subjects

Baoling Huang

Publications and source records attributed to Baoling Huang.

14 recordsLinked to original sources

arXiv2026

Machine Learning-Guided Screening of Advantageous Solvents for Solid Polymer Electrolytes in Lithium Metal Batteries

Trace residual solvents in solid polymer electrolytes (SPEs) significantly affect electrolyte and interface properties, where optimal selection enhances ionic conductivity and transference numbers. However, solvent complexity hinders general screening methods. We establish a universal criterion linking electronic (HOMO, LUMO) and macroscopic properties (dielectric constant, dipole moment, polarizability) via machine learning on an approximately 10,000-solvent dataset from high-throughput DFT. Two solvents, N-methoxy-N-methyl-2,2,2-trifluoroacetamide and 2,2,2-trifluoro-N,N-dimethylacetamide, were identified. Experimental incorporation of trace N-methoxy-N-methyl-2,2,2-trifluoroacetamide into a poly(vinylidene fluoride-co-hexafluoropropylene) matrix achieves a 4.5 V window, 5.5x10^-4 S cm^-1 conductivity (30 C), and 0.78 Li+ transference number. The cell retains 86.7% capacity over 500 cycles (LiFePO4) and 98.7% after 200 cycles at 2C (LiNi0.9Co0.05Mn0.05O2), outperforming 2,2,2-trifluoro-N,N-dimethylacetamide, dimethylformamide, N-methyl-2-pyrrolidone, and dimethyl sulfoxide. This synergy enables balanced ion transport, wide stability, and cycling durability, advancing safer, high-energy lithium metal batteries. Our integrated approach establishes a solvent screening paradigm for rational SPE design, accelerating next-generation battery development.

cond-mat.mtrl-sci↗

arXiv2024

Ineffectiveness of Formamidine in Suppressing Ultralow Thermal Conductivity in Cubic Hybrid Perovskite FAPbI3

Fundamentally understanding the lattice dynamics and microscopic mechanisms of thermal transport in cubic hybrid organic-inorganic perovskites remains elusive, primarily due to their strong anharmonicity and frequent phase transitions. In this work, we comprehensively investigate the thermal transport behavior in cubic hybrid perovskite FAPbI3, integrating first principles-based anharmonic lattice dynamics with a linearized Wigner transport formula. The Temperature Dependent Effective Potential (TDEP) technique allows us to stabilize the negative soft modes, primarily dominated by organic cations, at finite temperatures in cubic FAPbI3. We then predict an ultra-low thermal conductivity of ~0.63 Wm^(-1) K^(-1) in cubic FAPbI3 at 300 K, with a temperature dependence of T^(-0.740), suggesting a good crystalline nature of phonon transport. Notably, the ultra-low thermal conductivity in cubic FAPbI3 is primarily attributed to the [PbI3]1- units, challenging the conventional focus on organic FA+ cations. This shift in focus is due to the presence of Pb(s)-I(p) anti-bonding sates within the [PbI3]1- units. Furthermore, thermal transport in cubic FAPbI3 is predominantly governed by the particle-like phonon propagation channel across the entire temperature range of 300-500 K, a result of diminished suppression of low-frequency phonons by FA+ cations and large inter-branch spacings. Finally, our findings underscore that the anharmonic force constants are highly temperature-sensitive, leading to underestimations of thermal conductivity when relying on 0-K anharmonic force constants. Our study not only elucidates the microscopic mechanisms of thermal transport in cubic FAPbI3 but also provides a crucial framework for the discovery, design, and understanding of hybrid organic-inorganic compounds with ultra-low thermal conductivity.

cond-mat.mtrl-sci↗

arXiv2023

Infrared anomalies in ultrathin Ti3C2Tx MXene films

Visible transparent but infrared reflective materials are ideal candidates for both transparent conductive films and low-emissivity glass, which are highly desired in a broad variety of areas such as touchscreens and displays, photovoltaics, smart windows, and antistatic coatings. Ultrathin Ti3C2Tx MXene films are emerging as promising low-emissivity transparent candidates. However, the fundamental IR properties of Ti3C2Tx has not been revealed experimentally due to daunting challenges in the preparation of continuous, large-area, and ultrathin films of optical quality on flat substrates. Herein, we proposed a tape-free transfer method that can help prepare centimeter-size and ultrathin (down to 8 nm) Ti3C2Tx films on diverse optical substrates. Benefitting from this method, the refractive index and permittivity for Ti3C2Tx were successfully measured. Ti3C2Tx films exhibit large in-plane permittivity in the IR region, yielding maximum IR reflectance of 88% for bulk films. Interestingly, three anomalies were found in ultrathin Ti3C2Tx films: strong dispersion in the permittivity, interlayer space-dependent optical properties, and abnormally high IR absorption for a 15-nm-thick film. These anomalies are important guidelines in the design of Ti3C2Tx-based low-emissivity transparent films and other related devices, and may inspire other intriguing applications such as ultrathin IR absorption coatings and tunable IR optical devices.

cond-mat.mtrl-sci↗

arXiv2023

Wave-like Tunneling of Phonons Dominates Glass-like Thermal Transport in Quasi-1D Copper Halide CsCu2I3

Fundamental understanding of thermal transport in compounds with ultra-low thermal conductivity remains challenging, primarily due to the limitations of conventional lattice dynamics and heat transport models. In this study, we investigate the thermal transport in quasi-one-dimensional (1D) copper halide CsCu2I3 by employing a combination of first principles-based self-consistent phonon calculations and a dual-channel thermal transport model. Our results show that the 0-K unstable soft modes, primarily dominated by Cs and I atoms in CsCu2I3, can be an-harmonically stabilized at ~ 75 K. Furthermore, we predict an ultra-low thermal conductivity of 0.362 Wm^(-1) K^(-1) along the chain axis and 0.201 Wm^(-1) K^(-1) along cross chain direction in CsCu2I3 at 300 K. Importantly, we find that an unexpected anomalous trend of increasing cross-chain thermal conductivity with increasing temperature for CsCu2I3, following a temperature dependence of ~T 0.106, which is atypical for a single crystal and classified as an abnormal glass-like behavior. The peculiar temperature-dependent behavior of thermal conductivity is elucidated by the dominant wave-like tunnelling of phonons in thermal transport of CsCu2I3 along cross-chain direction. In contrast, particle-like phonon propagation primarily contributes to the chain-axis thermal conductivity across the entire temperature range of 300-700 K. The sharp difference in the dominant thermal transport channels between the two crystallographic directions can be attributed to the unique chain-like quasi-1D structure of CsCu2I3. Our study not only illustrates the microscopic mechanisms of thermal transport in CsCu2I3 but also paves the way for searching for and designing materials with ultra-low thermal conductivity.

cond-mat.mtrl-sci↗

arXiv2023

Unravelling Ultralow Thermal Conductivity in Double Perovskite Cs2AgBiBr6: Dominant Wave-like Phonon Tunnelling, Strong Quartic Anharmonicity and Lattice Instability

In this work, we investigate the microscopic mechanisms of anharmonic lattice dynamics and thermal transport in lead-free halide double perovskite Cs2AgBiBr6 from first principles. We combine self-consistent phonon calculations with bubble diagram correction and a unified theory of lattice thermal transport that considers both the particle-like phonon propagation and wave-like tunnelling of phonons. An ultra-low thermal conductivity at room temperature (~0.21 Wm-1K-1) is predicted with weak temperature dependence(~T-0.45), in sharp contrast to the conventional ~T-1 dependence. Particularly, the vibrational properties of Cs2AgBiBr6 are featured by strong anharmonicity and wave-like tunnelling of phonons. Anharmonic phonon renormalization from both the cubic and quartic anharmonicities are found essential in precisely predicting the phase transition temperature in Cs2AgBiBr6 while the negative phonon energy shifts induced by cubic anharmonicity has a significant influence on particle-like phonon propagation. Further, the contribution of the wave-like tunnelling to the total thermal conductivity surpasses that of the particle-like propagation above around 340 K, indicating the breakdown of the phonon gas picture conventionally used in the Peierls-Boltzmann Transport Equation. Importantly, further including four-phonon scatterings is required in achieving the dominance of wave-like tunnelling, as compared to the dominant particle-like propagation channel when considering only three-phonon scatterings. Our work highlights the importance of lattice anharmonicity and wave-like tunnelling of phonons in the thermal transport in lead-free halide double perovskites.

cond-mat.mtrl-sci↗

arXiv2022

Hybrid aqueous/ionic liquid electrolyte for high cycle stability and low temperature adaptability lithium-ion battery

Aqueous rechargeable batteries are promising energy storage devices for the high safety, environmental friendliness, and easy assembly. However, their cycle stability and low temperature performance are limited by the narrow electrochemical stability window and the high freezing point of the aqueous electrolytes. Here, a hybrid electrolyte with a wide electrochemical window (2.15V) and a low freezing point (-60 oC) is developed by using EMIMDep as a novel additive. The hydrophobic EMIM+ accumulates on the negatively charged electrode and repels the water molecules, thus suppressing the water splitting. Meanwhile, the hydrophilic Dep- forms strong hydrogen bonds with water, thereby reducing the freezing point of the electrolyte. In addition, the hybrid 1 M LiNO3 in EMIMDep20-H2O80 electrolytes exhibit high safety and high stability due to the non-flammability, non-volatility, and low toxicity of the EMIMDep compared with other organic additives. Owing to the advantages of the aqueous/EMIMDep electrolyte, the full battery with LiTi$_2$(PO$_4$)$_3$ anode and LiMn$_2$O$_4$ cathode delivers an average voltage of 1.6 V and a specific capacity of 120 mAh/g with a capacity retention of 80% after 500 cycles at 1C. In addition, the full battery working at -35 oC delivers 60% specific capacity of that at room temperature.

physics.chem-ph↗

arXiv2022

Self-protecting aqueous lithium-ion batteries with smart ther-moresponsive separators

Capacity degradation and destructive hazards are two core challenges for lithium-ion batteries at high temperatures, which need to be solved urgently. Adding flame retardants or fire extinguishing agents can only achieve one-time self-protection in case of emergency overheating. Herein, smart self-protecting aqueous lithium-ion batteries were developed using thermoresponsive separators through in-situ polymerization on the hydrophilic separator. The thermoresponsive separator will close the lithium ions transport channel at high temperatures and reopen when the battery cools down; more importantly, the transition is reversible. We studied the lithium salts influence on the thermoresponsive properties of the hydrogels and selected suitable lithium salt (LiNO3) and concentration (1 M) in the electrolyte to achieve self-protection without sacrificing battery performance. In addition, the shut-off temperature can be tuned by adjusting the hydrophilic and hydrophobic moiety ratio in the hydrogel according to actual demands. This self-protecting lithium-ion battery shows promise for smart energy storage devices with safe and extended lifespan.

hep-ex↗

arXiv2021

Giant and bidirectionally tunable thermopower in non-aqueous ionogels enabled by selective ion doping

Ionic thermoelectrics show great potential in low-grade heat harvesting and thermal sensing owing to their ultrahigh thermopower, low cost and ease in production. However, the lack of effective n-type ionic thermoelectric materials seriously hinders their applications. Here, we report giant and bidirectionally tunable thermopowers within an ultrawide range from -23 to +32 mV K-1 at 90% RH in solid ionic-liquid-based ionogels, rendering it among the best n- and p-type ionic thermoelectric materials. A novel thermopower regulation strategy through ion doping to selectively induce ion aggregates via strong ion-ion interactions is proposed. These charged aggregates are found decisive in modulating the sign and enlarging the magnitude of the thermopower in the ionogels. A prototype wearable device integrated with 12 p-n pairs is demonstrated with a total thermopower of 0.358 V K-1 in general indoor conditions, showing promise for ultrasensitive body heat detection.

physics.app-ph↗

arXiv2021

2D MXenes: Visible Black but Infrared White Materials

Black materials with low infrared absorption/emission (or IR white) are rare in nature but highly desired in numerous areas, such as solar-thermal energy harvesting, multispectral camouflage, thermal insulation, and anti-counterfeiting. Due to the lack of spectral selectivity in intrinsic materials, such counter-intuitive properties are generally realized by constructing complicated subwavelength metamaterials with costly nanofabrication techniques. Here we report the low mid-IR emissivity (down to 10%) of 2D Ti3C2Tx MXenes. Associated with a high solar absorptance (up to 90%), they embrace the best spectral selectivity among the reported intrinsic black solar absorbing materials. Their appealing potentials in several aforementioned areas are experimentally demonstrated. First-principles calculations reveal that the IR emissivity of MXenes relies on both the nanoflake orientations and terminal groups, indicating great tunability. The calculations also suggest that more MXenes including Ti2CTx, Nb2CTx, and V2CTx are also potential low-emissivity materials. This work opens the avenue to further exploration of a family of intrinsically low-emissivity materials with over 70 members.

cond-mat.mtrl-sci↗

arXiv2017

Generalized two-temperature model for coupled phonons

The design of graphene-based composite with high thermal conductivity requires a comprehensive understanding of phonon coupling in graphene. We extended the two-temperature model to coupled groups of phonon. The study give new physical quantities, the phonon-phonon coupling factor and length, to characterize the couplings quantitatively. Besides, our proposed coupling length has an obvious dependence on system size. Our studies can not only observe the nonequilibrium between different groups of phonon, but explain theoretically the thermal resistance inside graphene.

cond-mat.mes-hall↗

arXiv2017

Further improvement of lattice thermal conductivity from bulk crystalline to 1-D-chain polyethylene: A high-yet-finite thermal conductivity using first-principles calculation

We calculate the thermal conductivity (\k{appa}) of both bulk crystalline and single-chain polyethylene (PE) using the first-principles-based anharmonic lattice dynamics. Despite its low \k{appa} in amorphous state, the predicted bulk crystal has high axial \k{appa} (237 W/m-K) at room temperature. The much lower measured \k{appa} is attributed to the small size of nanocrystallites (~10 nm) in synthesized semi-crystalline PE. For the 1-D chain, the predicted \k{appa} is much larger and yet finite (1400 W/m-K at room temperature). The reduction of scattering phase space caused by the diminished interchain van der Waals interactions explains this larger \k{appa}. It is also found that the transverse phonon branches with quadratic dispersion make minor contribution to this, due to their vanishing group velocity in the long-wavelength limit. Moreover, the low-frequency bending and twisting phonon modes are strongly coupled and dominate anharmonic phonon scatterings, leading to the finite \k{appa}. The predicted high \k{appa} of bulk and chain PE crystals enable polymer usage in thermal management and the above phonon scatterings provide guide for their nano-designs.

cond-mat.mes-hall↗

arXiv2015

First-principles study of anisotropic thermoelectric transport properties of IV-VI semiconductor compounds SnSe and SnS

We conduct comprehensive investigations of both thermal and electrical transport properties of SnSe and SnS using first-principles calculations combined with the Boltzmann transport theory. Due to the distinct layered lattice structure, SnSe and SnS exhibit similarly anisotropic thermal and electrical behaviors. The cross-plane lattice thermal conductivity $κ_{L}$ is 40-60% lower than the in-plane values. Extremely low $κ_{L}$ is found for both materials because of high anharmonicity. It is suggested that nanostructuring would be difficult to further decrease $κ_{L}$ because of the short mean free paths of dominant phonon modes (1-30 nm at 300 K) while alloying would be efficient in reducing $κ_{L}$ considering that the relative $κ_{L}$ contribution ($\sim$ 65%) of optical phonons is remarkably large. On the electrical side, the anisotropic electrical conductivities are mainly due to the different effective masses of holes and electrons along the $a$, $b$ and $c$ axes. This leads to the highest optimal $ZT$ values along the $b$ axis and lowest ones along the $a$ axis in both $p$-type materials. However, the $n$-type ones exhibit the highest $ZT$s along the $a$ axis due to the enhancement of power factor when the chemical potential gradually approaches the secondary band valley that causes significant increase in electron mobility and density of states. SnSe exhibits larger optimal $ZT$s compared with SnS in both $p$-type and $n$-type materials. For both materials, the peak $ZT$s of $n$-type materials are much higher than those of $p$-type ones along the same direction. The predicted highest $ZT$ values at 750 K are 1.0 in SnSe and 0.6 in SnS along the $b$ axis for the $p$-type doping while those for the $n$-type doping reach 2.7 in SnSe and 1.5 in SnS along the $a$ axis, rendering them among the best bulk thermoelectric materials for large-scale applications.

cond-mat.mtrl-sci↗

arXiv2015

Thermal conductivity of graphene mediated by strain and size

Based on first-principles calculations and full iterative solution of the linearized Boltzmann-Peierls transport equation for phonons within three-phonon scattering framework, we characterize the lattice thermal conductivities $κ$ of strained and unstrained graphene. We find $κ$ converges to 5450 W/m-K for infinite unstrained graphene, while $κ$ diverges for strained graphene with increasing system size at room temperature. The different $κ$ behaviors for these systems are further validated mathematically through phonon lifetime analysis. Flexural acoustic phonons are the dominant heat carriers in both unstrained and strained graphene within the temperature considered. Ultralong mean free paths of flexural phonons contribute to finite size effects on $κ$ for samples as large as 8 cm at room temperature. The calculated size-dependent and temperature-dependent $κ$ for finite samples agree well with experimental data, demonstrating the ability of the present approach to predict $κ$ of larger graphene sample. Tensile strain hardens the flexural modes and increases their lifetimes, causing interesting dependence of $κ$ on sample size and strain due to the competition between boundary scattering and intrinsic phonon-phonon scattering. These findings shed light on the nature of thermal transport in two-dimensional materials and may guide predicting and engineering $κ$ of graphene by varying strain and size.

cond-mat.mtrl-sci↗

arXiv2014

Enhanced thermoelectric figure-of-merit in boron-doped SiGe thin films by nanograin boundaries

Boron-doped polycrystalline silicon-germanium (SiGe) thin films are grown by low-pressure chemical vapor deposition (LPCVD) and their thermoelectric properties are characterized from 120 K to 300 K for the potential applications in integrated microscale cooling. The naturally formed grain boundaries are found to play a crucial role in determining both the charge and thermal transport properties of the films. Particularly, the unique columnar grain structures result in remarkable thermal conductivity anisotropy with the in-plane thermal conductivities of SiGe films about 50% lower than the cross-plane values. By optimizing the growth conditions and doping level, a high figure of merit (ZT) of 0.2 for SiGe films is achieved at 300 K, which is about 100% higher than the previous record for p-type SiGe alloys, mainly due to the significant reduction in the in-plane thermal conductivity caused by nanograin boundaries. The low cost and excellent scalability of LPCVD render these high-performance SiGe films ideal candidates for thin-film thermoelectric applications.

cond-mat.mtrl-sci↗