A. James Clark School of Engineering

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    ELECTRIFIED HIGH-TEMPERATURE MANUFACTURING AND APPLICATIONS IN ENVIRONMENTAL SCIENCE
    (2023) Li, Shuke; Hu, Liangbing; Material Science and Engineering; Digital Repository at the University of Maryland; University of Maryland (College Park, Md.)
    High temperature processes hold great potential for material and chemical manufacturing.On the one hand, high temperature can help overcome energy barriers and thus effectively convert precursors to desired products. On the other hand, high temperature can also boost the reaction rate and improve synthesis efficiency. Recent development of electrified high temperature technologies by our group further revealed the important role played by non-equilibrium conditions on nanomaterial and chemical syntheses. For example, Joule-heating of carbon-based materials through a programmable electrical signal can offer spatial and temporal temperature profiles, which can be used to manipulate the chemical reaction pathways. For another example, tunable heating duration and quenching rates can be used to achieve a range of compositions and structures of nanoparticles. In this dissertation, two specific applications of the electrified high temperature technology will be explored, including: (1) Thermal shock synthesis of multielemental nanoparticles as selective and stable catalysts; and (2) Efficient biomass upgrading via pulsed electrical heating. Supported nanoparticle (NP) catalysts are widely used for various reactions. However, it remains challenging to synthesize high quality NPs with accurate morphologically and structure control. In this part of the research, NP catalysts with morphology or structural design were prepared by high temperature thermal shock methods. Ultra-small and high-loading carbon supported Pt3Ni NPs: Strong electrostatic effect was introduced between metal salts and carbon particles that can largely improve anchoring and dispersion of the precursors, thereby achieving high NP loading (40 wt%) as well as small NP size and good distribution (1.66 ± 0.56 nm). This method is not only limited to bimetallic NPs synthesis or NPs on carbon black but can be extended to a range of NP compositions on various substrate materials, thus providing a general strategy for developing ultrafine and high-loading NPs as electrocatalysts for various reactions. Sustainable aviation fuels (SAFs) are essential to meet future air travel demand while reducing the carbon footprint. Among many potential feedstocks to produce SAFs, lignin stands out as it is an abundant and renewable aromatic biopolymer that is usually treated as a waste material from the paper industry. However, converting lignin to SAFs by conventional thermochemical processes has been challenging due to poor control on the reaction pathway which leads to undesired product distribution. In this study, a programmed electrified heating method was designed and used to break down large lignin molecule to small aromatic molecules with targeted product distribution. A controlled heating step offers sufficient energy input to break down lignin molecules to smaller fragments without excessive secondary reactions toward undesired species such as coke. The lignin thermal decomposition products were evaluated as potential precursor for SAFs generation. This process can be further extended to process other biomass materials such as algae and sawdust to value-added chemicals.
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    Direct and Rapid High-Temperature Upcycling of Degraded Graphite
    (Wiley, 2023-06-27) Li, Tangyuan; Tao, Lei; Xu, Lin; Meng, Taotao; Clifford, Bryson Callie; Li, Shuke; Zhao, Xinpeng; Rao, Jiancun; Lin, Feng; Hu, Liangbing
    Recycling the degraded graphite is becoming increasingly important, which can helped conserve natural resources, reduce waste, and provide economic and environmental benefits. However, current regeneration methods usually suffer from the use of harmful chemicals, high energy and time consumption, and poor scalability. Herein, we report a continuously high-temperature heating (≈2000 K) process to directly and rapidly upcycle degraded graphite containing impurities. A sloped carbon heater is designed to provide the continuous heating source, which enables robust control over the temperature profile, eliminating thermal barrier for heat transfer compared to conventional furnace heating. The upcycling process can be completed within 0.1 s when the degraded graphite rolls down the sloped heater, allowing us to produce the upcycled graphite on a large scale. High-temperature heating removes impurities and enhances the graphitization degree and (002) interlayer spacing, making the upcycled graphite more suitable for lithium intercalation and deintercalation. The assembled upcycled graphite||Li cell displays a high reversible capacity of ≈320 mAh g−1 at 1 C with a capacity retention of 96% after 500 cycles, comparable to current state-of-the-art recycled graphite. The method is a chemical-free, rapid, and scalable way to upcycle degraded graphite, and is adaptable to recycle other electrode materials.
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    Ultrahigh-Temperature Melt Printing of Multi-Principal Element Alloys
    (Nature Portfolio, 2022-11-07) Wang, Xizheng; Zhao, Yunhao; Chen, Gang; Zhao, Xinpeng; Liu, Chuan; Sridar, Soumya; Pizano, Luis Fernando Ladinos; Li, Shuke; Brozena, Alexandra H.; Guo, Miao; Zhang, Hanlei; Wang, Yuankang; Xiong, Wei; Hu, Liangbing
    Multi-principal element alloys (MPEA) demonstrate superior synergetic properties compared to single-element predominated traditional alloys. However, the rapid melting and uniform mixing of multi-elements for the fabrication of MPEA structural materials by metallic 3D printing is challenging as it is difficult to achieve both a high temperature and uniform temperature distribution in a sufficient heating source simultaneously. Herein, we report an ultrahigh-temperature melt printing method that can achieve rapid multielemental melting and uniform mixing for MPEA fabrication. In a typical fabrication process, multi-elemental metal powders are loaded into a hightemperature column zone that can be heated up to 3000 K via Joule heating, followed by melting on the order of milliseconds and mixing into homogenous alloys, which we attribute to the sufficiently uniform high-temperature heating zone. As proof-of-concept, we successfully fabricated single-phase bulk NiFeCrCo MPEA with uniform grain size. This ultrahigh-temperature rapid melt printing process provides excellent potential toward MPEA 3D printing