Xiaolin Zheng, Postdoctoral Faculty Sponsor
Effect of grain size on iron-boride nanoglasses
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
2023; 141: 116-123
View details for DOI 10.1016/j.jmst.2022.09.025
View details for Web of Science ID 000890718200004
Do we need perfect mixing between fuel and oxidizer to maximize the energy release rate of energetic nanocomposites?
APPLIED PHYSICS LETTERS
2023; 122 (1)
View details for DOI 10.1063/5.0133995
View details for Web of Science ID 000909857500002
Hydrogen-substituted graphdiyne-assisted ultrafast sparking synthesis of metastable nanomaterials.
Metastable nanomaterials, such as single-atom and high-entropy systems, with exciting physical and chemical properties are increasingly important for next-generation technologies. Here, we developed a hydrogen-substituted graphdiyne-assisted ultrafast sparking synthesis (GAUSS) platform for the preparation of metastable nanomaterials. The GAUSS platform can reach an ultra-high reaction temperature of 3,286K within 8ms, a rate exceeding 105Ks-1. Controlling the composition and chemistry of the hydrogen-substituted graphdiyne aerogel framework, the reaction temperature can be tuned from 1,640 K to 3,286K. We demonstrate the versatility of the GAUSS platform with the successful synthesis of single atoms, high-entropy alloys and high-entropy oxides. Electrochemical measurements and density functional theory show that single atoms synthesized by GAUSS enhance the lithium-sulfur redox reaction kinetics in all-solid-state lithium-sulfur batteries. Our design of the GAUSS platform offers a powerful way to synthesize a variety of metastable nanomaterials.
View details for DOI 10.1038/s41565-022-01272-4
View details for PubMedID 36585516
Author Correction: Discovery of LaAlO3 as an efficient catalyst for two-electron water electrolysis towards hydrogen peroxide.
2022; 13 (1): 7685
View details for DOI 10.1038/s41467-022-35478-w
View details for PubMedID 36509777
Discovery of LaAlO3 as an efficient catalyst for two-electron water electrolysis towards hydrogen peroxide.
2022; 13 (1): 7256
Electrochemical two-electron water oxidation reaction (2e-WOR) has drawn significant attention as a promising process to achieve the continuous on-site production of hydrogen peroxide (H2O2). However, compared to the cathodic H2O2 generation, the anodic 2e-WOR is more challenging to establish catalysts due to the severe oxidizing environment. In this study, we combine density functional theory (DFT) calculations with experiments to discover a stable and efficient perovskite catalyst for the anodic 2e-WOR. Our theoretical screening efforts identify LaAlO3 perovskite as a stable, active, and selective candidate for catalyzing 2e-WOR. Our experimental results verify that LaAlO3 achieves an overpotential of 510mV at 10mAcm-2 in 4M K2CO3/KHCO3, lower than those of many reported metal oxide catalysts. In addition, LaAlO3 maintains a stable H2O2 Faradaic efficiency with only a 3% decrease after 3h at 2.7V vs. RHE. This computation-experiment synergistic approach introduces another effective direction to discover promising catalysts for the harsh anodic 2e-WOR towards H2O2.
View details for DOI 10.1038/s41467-022-34884-4
View details for PubMedID 36433962
Perfluoroalkyl-Functionalized Graphene Oxide as a Multifunctional Additive for Promoting the Energetic Performance of Aluminum.
Aluminum (Al) is a widely used metal fuel for energetic applications ranging from space propulsion and exploration, and materials processing, to power generation for nano- and microdevices due to its high energy density and earth abundance. Recently, the ignition and combustion performance of Al particles were found to be improved by graphene-based additives, such as graphene oxide (GO) and graphene fluoride (GF), as their reactions provide heat to accelerate Al oxidation, gas to reduce particle agglomeration, and fluorine-containing species to remove Al2O3. However, GF is not only expensive but also hydrophobic with poor mixing compatibility with Al particles. Herein, we report a multifunctional graphene-based additive for Al combustion, i.e., perfluoroalkyl-functionalized graphene oxide (CFGO), which integrates the benefits of GO and GF in one material. We compared the effects of CFGO to GO and GF on the ignition and combustion properties of nAl particles using thermogravimetric analysis, differential scanning calorimetry, temperature-jump ignition), Xe flash ignition, and constant-volume combustion test. These experiments confirm that CFGO generates fluorine-containing species, heat, and gases, which collectively lower the ignition threshold, augment the energy release rate, and reduce the combustion product agglomeration of nanosized Al particles, outperforming both GO and GF as additives. This work shows the great potential of using multifunctionalized graphene as an integrated additive for enhancing the ignition and combustion of metals.
View details for DOI 10.1021/acsnano.2c05271
View details for PubMedID 36099637
Ignition and combustion of Perfluoroalkyl-functionalized aluminum nanoparticles and nanothermite
COMBUSTION AND FLAME
View details for DOI 10.1016/j.combustflame.2022.112170
View details for Web of Science ID 000831314000007
Efficient and Stable Acidic Water Oxidation Enabled by Low-Concentration, High-Valence Iridium Sites
ACS ENERGY LETTERS
View details for DOI 10.1021/acsenergylett.2c00578
View details for Web of Science ID 000821179900001
Effect of Fluoroalkylsilane Surface Functionalization on Boron Combustion.
ACS applied materials & interfaces
Boron has been regarded as a promising high-energy fuel due to its high volumetric and gravimetric heating values. However, it remains challenging for boron to attain its theoretical heat of combustion because of the existence of its native boron oxide layer and its high melting and boiling temperatures that delay ignition and inhibit complete combustion. Boron combustion is known to be enhanced by physically adding fluorine-containing chemicals, such as fluoropolymer or metal fluorides, to remove surface boron oxides. Herein, we chemically functionalize the surface of boron particles with three different fluoroalkylsilanes: FPTS-B (F3-B), FOTS-B (F13-B), and FDTS-B (F17-B). We evaluated the ignition and combustion properties of those three functionalized boron particles as well as pristine ones. The boron particles functionalized with the longest fluorocarbon chain (F17) exhibit the most powerful energetic performance, the highest heat of combustion, and the strongest BO2 emission among all samples. These results suggest that the surface functionalization with fluoroalkylsilanes is an efficient strategy to enhance boron ignition and combustion.
View details for DOI 10.1021/acsami.2c00347
View details for PubMedID 35467848
Ultrahigh-Quality Infrared Polaritonic Resonators Based on Bottom-Up-Synthesized van der Waals Nanoribbons.
van der Waals nanomaterials supporting phonon polariton quasiparticles possess extraordinary light confinement capabilities, making them ideal systems for molecular sensing, thermal emission, and subwavelength imaging applications, but they require defect-free crystallinity and nanostructured form factors to fully showcase these capabilities. We introduce bottom-up-synthesized alpha-MoO3 structures as nanoscale phonon polaritonic systems that feature tailorable morphologies and crystal qualities consistent with bulk single crystals. alpha-MoO3 nanoribbons serve as low-loss hyperbolic Fabry-Perot nanoresonators, and we experimentally map hyperbolic resonances over four Reststrahlen bands spanning the far- and mid-infrared spectral range, including resonance modes beyond the 10th order. The measured quality factors are the highest from phonon polaritonic van der Waals structures to date. We anticipate that bottom-up-synthesized polaritonic van der Waals nanostructures will serve as an enabling high-performance and low-loss platform for infrared optical and optoelectronic applications.
View details for DOI 10.1021/acsnano.1c10489
View details for PubMedID 35041379
Ultrahigh-quality van der Waals hyperbolic polariton resonators
SPIE-INT SOC OPTICAL ENGINEERING. 2022
View details for DOI 10.1117/12.2612301
View details for Web of Science ID 000836330700010
Probing boron thermite energy release at rapid heating rates
COMBUSTION AND FLAME
View details for DOI 10.1016/j.combustflame.2021.111491
View details for Web of Science ID 000759564400008
High thermoelectric figure of merit of porous Si nanowires from 300 to 700K.
2021; 12 (1): 3926
Thermoelectrics operating at high temperature can cost-effectively convert waste heat and compete with other zero-carbon technologies. Among different high-temperature thermoelectrics materials, silicon nanowires possess the combined attributes of cost effectiveness and mature manufacturing infrastructures. Despite significant breakthroughs in silicon nanowires based thermoelectrics for waste heat conversion, the figure of merit (ZT) or operating temperature has remained low. Here, we report the synthesis of large-area, wafer-scale arrays of porous silicon nanowires with ultra-thin Si crystallite size of ~4nm. Concurrent measurements of thermal conductivity (kappa), electrical conductivity (sigma), and Seebeck coefficient (S) on the same nanowire show a ZT of 0.71 at 700K, which is more than ~18 times higher than bulk Si. This ZT value is more than two times higher than any nanostructured Si-based thermoelectrics reported in the literature at 700K. Experimental data and theoretical modeling demonstrate that this work has the potential to achieve a ZT of ~1 at 1000K.
View details for DOI 10.1038/s41467-021-24208-3
View details for PubMedID 34168136
Enhancing Mechanical and Combustion Performance of Boron/Polymer Composites via Boron Particle Functionalization.
ACS applied materials & interfaces
High-speed air-breathing propulsion systems, such as solid fuel ramjets (SFRJ), are important for space exploration and national security. The development of SFRJ requires high-performance solid fuels with excellent mechanical and combustion properties. One of the current solid fuel candidates is composed of high-energy particles (e.g., boron (B)) and polymeric binder (e.g., hydroxyl-terminated polybutadiene (HTPB)). However, the opposite polarities of the boron surface and HTPB lead to poor B particle dispersion and distribution within HTPB. Herein, we demonstrate that the surface functionalization of B particles with nonpolar oleoyl chloride greatly improves the dispersion and distribution of B particles within HTPB. The improved particle dispersion is quantitatively visualized through X-ray computed tomography imaging, and the particle/matrix interaction is evaluated by dynamic mechanical analysis. The surface-functionalized B particles can be uniformly dispersed up to 40 wt % in HTPB, the highest mass loading reported to date. The surface-functionalized B (40 wt %)/HTPB composite exhibits a 63.3% higher Young's modulus, 87.5% higher tensile strength, 16.2% higher toughness, and 16.8% higher heat of combustion than pristine B (40 wt %)/HTPB. The surface functionalization of B particles provides an effective strategy for improving the efficacy and safety of B/HTPB solid fuels for future high-speed air-breathing vehicles.
View details for DOI 10.1021/acsami.1c06727
View details for PubMedID 34110148
Ultrahigh Doping of Graphene Using Flame-Deposited MoO3
IEEE ELECTRON DEVICE LETTERS
2020; 41 (10): 1592–95
View details for DOI 10.1109/LED.2020.3018485
View details for Web of Science ID 000573814300034
Enhancing combustion performance of nano-Al/PVDF composites with beta-PVDF
COMBUSTION AND FLAME
2020; 219: 467–77
View details for DOI 10.1016/j.combustflame.2020.06.011
View details for Web of Science ID 000564899700003
On-demand production of hydrogen by reacting porous silicon nanowires with water
View details for DOI 10.1007/s12274-020-2734-8
View details for Web of Science ID 000521006500001
Synergistically Chemical and Thermal Coupling between Graphene Oxide and Graphene Fluoride for Enhancing Aluminum Combustion.
ACS applied materials & interfaces
Metal combustion reaction is highly exothermic and is used in energetic applications, such as propulsion, pyrotechnics, powering micro- and nano-devices, and nanomaterials synthesis. Aluminum (Al) is attracting great interest in those applications because of its high energy density, earth abundance, and low toxicity. Nevertheless, Al combustion is hard to initiate and progresses slowly and incompletely. On the other hand, ultrathin carbon nanomaterials, such as graphene, graphene oxide (GO), and graphene fluoride (GF), can also undergo exothermic reactions. Herein, we demonstrate that the mixture of GO and GF significantly improves the performance of Al combustion as interactions between GO and GF provide heat and radicals to accelerate Al oxidation. Our experiments and reactive molecular dynamics simulation reveal that GO and GF have strong chemical and thermal couplings through radical reactions and heat released from their oxidation reactions. GO facilitates the dissociation of GF, and GF accelerates the disproportionation and oxidation of GO. When the mixture of GO and GF is added to micron-sized Al particles, their synergistic couplings generate reactive oxidative species, such as CF x and CF x O y , and heat, which greatly accelerates Al combustion. This work demonstrates a new area of using synergistic couplings between ultrathin carbon nanomaterials to accelerate metal combustion and potentially oxidation reactions of other materials.
View details for DOI 10.1021/acsami.9b20397
View details for PubMedID 31950820
Experimental effective metal oxides to enhance boron combustion
COMBUSTION AND FLAME
2019; 205: 278–85
View details for DOI 10.1016/j.combustflame.2019.04.018
View details for Web of Science ID 000471742000026
Modified Micro-Emulsion Synthesis of Highly Dispersed Al/PVDF Composites with Enhanced Combustion Properties
ADVANCED ENGINEERING MATERIALS
2019; 21 (5)
View details for DOI 10.1002/adem.201801330
View details for Web of Science ID 000473099800022
Tuning the morphological, ignition and combustion properties of micron-Al/CuO thermites through different synthesis approaches
COMBUSTION AND FLAME
2018; 195: 303–10
View details for DOI 10.1016/j.combustflame.2018.04.028
View details for Web of Science ID 000440118500027
Enhanced interfacial bonding and mechanical properties in CNT/Al composites fabricated by flake powder metallurgy
2018; 130: 333-339
View details for DOI 10.1016/j.carbon.2018.01.037
Energetic Performance of Optically Activated Aluminum/Graphene Oxide Composites.
Optical ignition of solid energetic materials, which can rapidly release heat, gas, and thrust, is still challenging due to the limited light absorption and high ignition energy of typical energetic materials ( e.g., aluminum, Al). Here, we demonstrated that the optical ignition and combustion properties of micron-sized Al particles were greatly enhanced by adding only 20 wt % of graphene oxide (GO). These enhancements are attributed to the optically activated disproportionation and oxidation reactions of GO, which release heat to initiate the oxidization of Al by air and generate gaseous products to reduce the agglomeration of the composites and promote the pressure rise during combustion. More importantly, compared to conventional additives such as metal oxides nanoparticles ( e.g., WO3 and Bi2O3), GO has much lower density and therefore could improve energetic properties without sacrificing Al content. The results from Xe flash ignition and laser-based excitation experiments demonstrate that GO is an efficient additive to improve the energetic performance of micron-sized Al particles, enabling micron-sized Al to be ignited by optical activation and promoting the combustion of Al in air.
View details for DOI 10.1021/acsnano.8b06217
View details for PubMedID 30335365
Electroless Deposition and Ignition Properties of Si/Fe2O3 Core/Shell Nanothermites.
2017; 2 (7): 3596-3600
Thermite, a composite of metal and metal oxide, finds wide applications in power and thermal generation systems that require high-energy density. Most of the researches on thermites have focused on using aluminum (Al) particles as the fuel. However, Al particles are sensitive to electrostatic discharge, friction, and mechanical impact, imposing a challenge for the safe handling and storage of Al-based thermites. Silicon (Si) is another attractive fuel for thermites because of its high-energy content, thin native oxide layer, and facile surface functionality. Several studies showed that the combustion properties of Si-based thermites are comparable to those of Al-based thermites. However, little is known about the ignition properties of Si-based thermites. In this work, we determined the reaction onset temperatures of mechanically mixed (MM) Si/Fe2O3 nanothermites and Si/Fe2O3 core/shell (CS) nanothermites using differential scanning calorimetry. The Si/Fe2O3 CS nanothermites were prepared by an electroless deposition method. We found that the Si/Fe2O3 CS nanoparticles (NPs) had a lower reaction onset temperature (∼550 °C) than the MM Si/Fe2O3 nanothermites (>650 °C). The onset temperature of the Si/Fe2O3 CS nanothermites is also insensitive to the size of the Si core NP. These results indicate that the interfacial contact quality between Si and Fe2O3 is the dominant factor for determining the ignition properties of thermites. Finally, the reaction onset temperature of the Si/Fe2O3 CS NPs is comparable to that of the commonly used Al-based nanothermites, suggesting that Si is an attractive fuel for thermites.
View details for DOI 10.1021/acsomega.7b00652
View details for PubMedID 31457677
View details for PubMedCentralID PMC6641388