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Zhang, Hanrui

Publications and source records attributed to Zhang, Hanrui.

6 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Bipolar Membrane Capacitive Deionization for the Selective Capture of Lithium Ions from Brines and Conversion to Lithium Hydroxide

Meeting the increasing demand for lithium in vehicle electrification and renewable energy storage requires innovations in lithium-ion (Li + ) separations. Traditional solar evaporation methods for lithium recovery are slow and consume tremendous volumes of water and secondary chemicals (acids and bases). This study introduces a bipolar membrane capacitive deionization (BPM-CDI) unit for direct lithium extraction and LiOH production without the external addition of acids and bases. Utilizing de-lithiated lithium-iron-phosphate (LFP) coated carbon cloth electrodes, the BPM-CDI unit demonstrates selective Li + capture over competing ions. Molecular dynamics simulations and H-cell experiments elucidate pH inversion mechanisms during Li + release, yielding LiOH. The BPM-CDI platform efficiently removes Li + from synthetic brines featuring 8x higher Mg 2+ concentrations (200 ppm Mg 2+ ) and 26x higher Na + concentrations (682 ppm Na + ), achieving a LiOH concentration of 124 ppm (36 ppm Li + ) after 8 cycles of recirculation. Post-mortem analysis confirms electrode integrity and stability. BPM-CDI integrated with selective electrodes is a promising electrochemical separation-reactor platform for lithium recovery while producing LiOH.

Kulkarni, Tanmay↗
DOE OSTI2024

Direct extraction of lithium from ores by electrochemical leaching

With the rapid increase in lithium consumption for electric vehicle applications, its price soared during the past decade. To secure a reliable and cost-effective supply chain, it is critical to unlock alternative lithium extraction resources beyond conventional brine. In this study, we develop an electrochemical method to directly leach lithium from α-phase spodumene. We find the H 2 O 2 promoter can significantly reduce the leaching potential by facilitating the electron transfer and changing the reaction path. Upon leaching, β-phase spodumene shows a typical phase transformation to HAlSi 2 O 6 , while leached α-phase remains its original crystal phase with a lattice shrinkage. To demonstrate the scale-up potential of electrochemical leaching, we design a catalyst-modified high-throughput current collector for high loading of suspended spodumene, achieving a leaching current of 18 mA and a leaching efficiency of 92.2%. Electrochemical leaching will revolutionize traditional leaching and recycling processes by minimizing the environmental footprint and energy consumption.

25 ENERGY STORAGE↗
DOE OSTI2024

Solvent-Mediated, Reversible Ternary Graphite Intercalation Compounds for Extreme-Condition Li-Ion Batteries

Traditional Li-ion intercalation chemistry into graphite anode exclusively utilizes the co-intercalation-free or co-intercalation mechanism. The latter mechanism is based on ternary graphite intercalation compounds (t-GICs), where glyme solvents were explored and proved to deliver unsatisfied cyclability in LIBs. Herein, we report a novel intercalation mechanism, that is, in-situ synthesis of t-THF-GICs in the tetrahydrofuran (THF) electrolyte via a spontaneous, controllable reaction between binary-GICs and free THF molecules during initial graphite lithiation. The spontaneous transformation from b-GIC to t-GIC, which is different from conventional co-intercalation chemistry, is characterized and quantified via operando synchrotron X-ray and electrochemical analyses. The resulting t-GIC chemistry obviates the necessity for complete Li-ion desolvation, facilitating rapid kinetics and synchronous charge/discharge of graphite particles even under high current densities. Consequently, the graphite anode demonstrates unprecedented fast charging (1 min), dendrite-free low-temperature performance, and ultralong lifetimes exceeding 10,000 cycles. Full cells coupled with layered cathode, display remarkable cycling stability upon a 15-min charging and excellent rate capability even at -40 °C. Furthermore, our chemical strategies are shown to extend beyond Li-ion batteries to encompass Na-ion and K-ion batteries, underscoring their broad applicability. Our work contributes to the advancement of graphite intercalation chemistry and presents a low-cost, adaptable approach to achieving fast-charging and low-temperature batteries.

25 ENERGY STORAGE↗
DOE OSTI2020

Multi-scale stabilization of high-voltage LiCoO 2 enabled by nanoscale solid electrolyte coating

LiCoO 2 (LCO) possess a high theoretical specific capacity of 274 mAh g -1 , and currently LCO charged to 4.48 V with a capacity of ~190–195 mAh g -1 is penetrating the commercial markets. Scalable strategies to further enhance the performance of LCO are highly attractive. Here, we develop a scalable ball-milling and sintering method to tackle this long-standing challenge by modifying LCO surface with only 1.5–3.5% ceramic solid electrolyte nanoparticles, specifically Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) as an example. Consequently, the atomic-to-meso multiscale structural stabilities have been significantly improved, even with a high cut-off voltage of 4.5 V vs. Li/Li + , leading to excellent electrochemical stabilities. The nano-LAGP modified Li|LCO cell exhibits high discharge capacity of 196 mAh g -1 at 0.1 C, capacity retention of 88% over 400 cycles, and remarkably enhanced rate capability (163 mAh g -1 at 6 C). These results show significant improvement compared to the Li|LCO cells. The as-prepared graphite|LAGP-LCO full cells also show steady cycling with 80.4% capacity retention after 200 cycles with a voltage cut-off of 4.45 V. This work provides a simple and scalable approach to achieve stable cycling of LCO at high voltage with high energy density.

25 ENERGY STORAGE↗
DOE OSTI2020

Interfacial engineering for stabilizing polymer electrolytes with 4V cathodes in lithium metal batteries at elevated temperature

Poly (ethylene oxide) (PEO) polymer electrolytes are promising candidates for next-generation rechargeable lithium batteries. However, the poor interfacial stability between 4 V cathodes and PEO electrolytes impedes their applications in 4 V lithium batteries with high energy density. Here, we demonstrate a facile and effective strategy to enhance the interfacial stability by the synergy of Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 (LAGP) coating on the cathode surface, and salt combination in the electrolyte, even with a cut-off voltage of 4.25–4.4 V vs. Li + /Li. Nano-LAGP coated Li|PEO|LiCoO 2 cell delivers stable cycling with a capacity retention of 81.9%/400 cycles and 84.7%/200 cycles at 60 °C when charged to 4.25 and 4.3 V in pure polyether electrolyte, respectively. Steady cycling is also demonstrated at room temperature and with LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) cathode. This work offers a viable and scalable approach to improve the stability between PEO electrolytes and 4 V cathodes and open up new possibilities for practical application of 4 V lithium metal batteries.

25 ENERGY STORAGE↗