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1.
Nano Lett ; 24(5): 1729-1737, 2024 Feb 07.
Artigo em Inglês | MEDLINE | ID: mdl-38289279

RESUMO

Rechargeable hydrogen gas batteries, driven by hydrogen evolution and oxidation reactions (HER/HOR), are emerging grid-scale energy storage technologies owing to their low cost and superb cycle life. However, compared with aqueous electrolytes, the HER/HOR activities in nonaqueous electrolytes have rarely been studied. Here, for the first time, we develop a nonaqueous proton electrolyte (NAPE) for a high-performance hydrogen gas-proton battery for all-climate energy storage applications. The advanced nonaqueous hydrogen gas-proton battery (NAHPB) assembled with a representative V2(PO4)3 cathode and H2 anode in a NAPE exhibits a high discharge capacity of 165 mAh g-1 at 1 C at room temperature. It also efficiently operates under all-climate conditions (from -30 to +70 °C) with an excellent electrochemical performance. Our findings offer a new direction for designing nonaqueous proton batteries in a wide temperature range.

2.
Angew Chem Int Ed Engl ; 63(7): e202315931, 2024 Feb 12.
Artigo em Inglês | MEDLINE | ID: mdl-38050465

RESUMO

Rechargeable Li-Cl2 battery is a promising high energy density battery system. However, reasonable cycle life could only be achieved under low specific capacities due to the sluggish oxidation of LiCl to Cl2 . Herein, we propose an amine-functionalized covalent organic framework (COF) with catalytic activity, namely COF-NH2 , that significantly decreases the oxidation barrier of LiCl and accelerates the oxidation kinetics of LiCl in Li-Cl2 cell. The resulting Li-Cl2 cell using COF-NH2 (Li-Cl2 @COF-NH2 ) simultaneously exhibits low overpotential, ultrahigh discharge capacity up to 3500 mAh/g and a promoted utilization ratio of deposited LiCl at the first cycle (UR-LiCl) of 81.4 %, which is one of the highest reported values to date. Furthermore, the Li-Cl2 @COF-NH2 cell could be stably cycled for over 200 cycles when operating at a capacity of 2000 mAh/g at -20 °C with a Coulombic efficiency (CE) of ≈100 % and a discharge plateau of 3.5 V. Our superior Li-Cl2 batteries enabled by organocatalyst enlighten an arena towards high-energy storage applications.

3.
J Am Chem Soc ; 145(50): 27877-27885, 2023 Dec 20.
Artigo em Inglês | MEDLINE | ID: mdl-38053318

RESUMO

Rechargeable Li-Cl2 batteries are recognized as promising candidates for energy storage due to their ultrahigh energy densities and superior safety features. However, Li-Cl2 batteries suffer from a short cycle life and low Coulombic efficiency (CE) at a high specific cycling capacity due to a sluggish and insufficient Cl2 supply during the redox reaction. To achieve Li-Cl2 batteries with high discharge capacity and CE, herein, we propose and design an imine-functionalized porous organic nanocage (POC) to enrich Cl2 molecules. Based on density functional theory (DFT) calculations, the imine group sites in host cages strongly interact with Cl2 molecules, facilitating the rapid capture of Cl2. As a result, the output capacity of the Li-Cl2 battery using POC (Li-Cl2@POC) is significantly boosted, achieving an ultrahigh discharge capacity of 4000 mAh/g at ∼100% CE. Benefiting from the designed POC, the highest utilization ratio of deposited LiCl at the first cycle in the Li-Cl2@POC battery reaches as high as 85%, superior to all reported values. The Li-Cl2@POC battery exhibits excellent electrochemical performance even at low temperatures, delivering stable cycling over 200 cycles under a capacity of 2000 mAh/g at -20 °C with a voltage plateau of 3.5 V and an average CE of 99.7%. We also demonstrate that the Li-Cl2@POC cells can be assembled and well-operated in a dry room, showing advantages for mass production. Our designed POC promotes the practical deployment of rechargeable Li-Cl2 batteries.

4.
J Am Chem Soc ; 145(46): 25422-25430, 2023 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-37877747

RESUMO

Hydrogen-chlorine (H2-Cl2) fuel cells have distinct merits due to fast electrochemical kinetics but are afflicted by high cost, low efficiency, and poor reversibility. The development of a rechargeable H2-Cl2 battery is highly desirable yet challenging. Here, we report a rechargeable H2-Cl2 battery operating statically in a wide temperature ranging from -70 to 40 °C, which is enabled by a reversible Cl2/Cl- redox cathode and an electrocatalytic H2 anode. A hierarchically porous carbon cathode is designed to achieve effective Cl2 gas confinement and activate the discharge plateau of Cl2/Cl- redox at room temperature, with a discharge plateau at ∼1.15 V and steady cycling for over 500 cycles without capacity decay. Furthermore, the battery operation at an ultralow temperature is successfully achieved in a phosphoric acid-based antifreezing electrolyte, with a reversible discharge capacity of 282 mAh g-1 provided by the highly porous carbon at -70 °C and an average Coulombic efficiency of 91% for more than 300 cycles at -40 °C. This work offers a new strategy to enhance the reversibility of aqueous chlorine batteries for energy storage applications in a wide temperature range.

5.
Nano Lett ; 23(20): 9664-9671, 2023 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-37638682

RESUMO

Aqueous proton batteries (APBs) have emerged as one of the most promising batteries for large-scale energy storage technology. However, they usually show an undesirable electrochemical performance. Herein, we demonstrate a novel aqueous catalytic hydrogen gas powered organic proton (HOP) battery, which is driven by hydrogen evolution/oxidation redox reactions via commercial nanocatalysts on the anode and coordination/decoordination reactions of C═O with H+ on the cathode. The HOP battery shows an excellent rate capacity of 190.1 mAh g-1 at 1 A g-1 and 71.4 mAh g-1 at 100 A g-1. It also delivers a capacity of 96.6 mAh g-1 after 100000 cycles and operates at temperatures down to -70 °C. Moreover, the HOP battery is fabricated in a large-scale pouch cell with an extended capacity, exhibiting its potential for practical energy storage applications. This work provides new insights into the building of sustainable APBs, which will broaden the horizons of high-performance aqueous batteries.

6.
Angew Chem Int Ed Engl ; 62(40): e202308454, 2023 Oct 02.
Artigo em Inglês | MEDLINE | ID: mdl-37563746

RESUMO

Metallic zinc (Zn) is considered as one of the most attractive anode materials for the post-lithium metal battery systems owing to the high theoretical capacity, low cost, and intrinsic safety. However, the Zn dendrites and parasitic side reaction impede its application. Herein, we propose a new principle of regulating p-band center of metal oxide protective coating to balance Zn adsorption energy and migration energy barrier for effective Zn deposition and stripping. Experimental results and theoretical calculations indicate that benefiting from the uniform zincophilic nucleation sites and fast Zn transport on indium tin oxide (ITO), highly stable and reversible Zn anode can be achieved. As a result, the I-Zn symmetrical cell achieves highly reversible Zn deposition/stripping with an extremely low overpotential of 9 mV and a superior lifespan over 4000 h. The Cu/I-Zn asymmetrical cell exhibits a long lifetime of over 4000 cycles with high average coulombic efficiency of 99.9 %. Furthermore, the assembled I-Zn/AC full cell exhibits an excellent lifetime for 70000 cycles with nearly 100 % capacity retention. This work provides a general strategy and new insight for the construction of efficient Zn anode protection layer.

7.
JACS Au ; 3(2): 488-497, 2023 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-36873693

RESUMO

In conventional water electrolysis (CWE), the H2 and O2 evolution reactions (HER/OER) are tightly coupled, making the generated H2 and O2 difficult to separate, thus resulting in complex separation technology and potential safety issues. Previous efforts on the design of decoupled water electrolysis mainly concentrated on multi-electrode or multi-cell configurations; however, these strategies have the limitation of involving complicated operations. Here, we propose and demonstrate a pH-universal, two-electrode capacitive decoupled water electrolyzer (referred to as all-pH-CDWE) in a single-cell configuration by utilizing a low-cost capacitive electrode and a bifunctional HER/OER electrode to separate H2 and O2 generation for decoupling water electrolysis. In the all-pH-CDWE, high-purity H2 and O2 generation alternately occur at the electrocatalytic gas electrode only by reversing the current polarity. The designed all-pH-CDWE can maintain a continuous round-trip water electrolysis for over 800 consecutive cycles with an electrolyte utilization ratio of nearly 100%. As compared to CWE, the all-pH-CDWE achieves energy efficiencies of 94% in acidic electrolytes and 97% in alkaline electrolytes at a current density of 5 mA cm-2. Further, the designed all-pH-CDWE can be scaled up to a capacity of 720 C in a high current of 1 A for each cycle with a stable HER average voltage of 0.99 V. This work provides a new strategy toward the mass production of H2 in a facilely rechargeable process with high efficiency, good robustness, and large-scale applications.

8.
Nano Lett ; 23(6): 2295-2303, 2023 Mar 22.
Artigo em Inglês | MEDLINE | ID: mdl-36876971

RESUMO

Aluminum (Al) metal is an attractive anode material for next-generation rechargeable batteries, because of its low cost and high capacities. However, it brings some fundamental issues such as dendrites, low Coulombic efficiency (CE), and low utilization. Here, we propose a strategy for constructing an ultrathin aluminophilic interface layer (AIL) to regulate the Al nucleation and growth behaviors, which enables highly reversible and dendrite-free Al plating/stripping under high areal capacity. Metallic Al can maintain stable plating/stripping on the Pt-AIL@Ti for over 2000 h at 10 mAh cm-2 with an average CE of 99.9%. The Pt-AIL also enables reversible Al plating/stripping at a record high areal capacity of 50 mAh cm-2, which is 1-2 orders of magnitude higher than the previous studies. This work provides a valuable direction for further construction of high-performance rechargeable Al metal batteries.

9.
ACS Appl Mater Interfaces ; 15(1): 1021-1028, 2023 Jan 11.
Artigo em Inglês | MEDLINE | ID: mdl-36542843

RESUMO

Hydrogen gas batteries are regarded as one of the most promising rechargeable battery systems for large-scale energy storage applications due to their advantages of high rates and long-term cycle lives. However, the development of cost-effective and low-temperature-tolerant hydrogen gas batteries is highly desirable yet very challenging. Herein, we report a novel conductive polymer-hydrogen gas battery that is suitable for ultralow-temperature energy storage applications and consists of a hydrogen gas anode, a conductive polymer cathode using polyaniline (PANI) or polypyrrole as examples, and protonic acidic electrolytes. The PANI-H2 battery using 1 M H2SO4 as the electrolyte exhibits a capacity of 67 mA h/g, a remarkable rate up to 15 A/g, a Coulombic efficiency around 100%, and an ultra-long life of 10,000 cycles. Using the anti-freezing 9 M H3PO4 electrolyte, the PANI-H2 battery can operate well at temperatures down to -70 °C, which maintains ∼70% of the capacity at room temperature and shows an excellent cycle stability under -60 °C. Benefiting from the fast redox kinetics of both electrodes, this work demonstrates excellent rate performance and low-temperature feasibility of conductive polymer-H2 batteries, providing a new avenue for further development of low-cost and reliable polymer-H2 batteries for large-scale energy storage.

10.
Acta Biochim Biophys Sin (Shanghai) ; 54(5): 615-624, 2022 May 25.
Artigo em Inglês | MEDLINE | ID: mdl-35593476

RESUMO

Cellular energy metabolism dysregulation is associated with colorectal cancer (CRC) development and progression. Discoidin domain receptor 1a (DDR1a), one of the five DDR1 isoforms, is closely related to cell proliferation, invasion, and apoptosis in various tumors. Whether it participates in cellular metabolic reprogramming and regulates CRC initiation and progression remains unclear. In this study, we compared the expression of DDR1 in CRC tissues and adjacent tissues from 126 postoperative CRC samples. Moreover, lentivirus-mediated DDR1a overexpression and knockdown were performed in LoVo cells, and cell viability and proliferation were determined by CCK-8 and BrdU assays, respectively. Oxygen consumption rate, extracellular acidification rate, and lactate production were used to determine the effect of DDR1a on metabolic reprogramming. Clinically, CRC patients with high DDR1 expression had poor differentiation and were at an advanced TNM stage. DDR1a promoted LoVo cell proliferation, mitochondrial function, and extracellular acidification. Moreover, DDR1a knockdown inhibited intracellular lactic acid production in LoVo cells, while a pyruvate kinase inhibitor (diamide, 200 µM) significantly reversed this progression. Taken together, our results reveal that DDR1 plays a crucial role in maintaining intracellular environment homeostasis through metabolic reprogramming.


Assuntos
Proliferação de Células , Neoplasias Colorretais , Receptor com Domínio Discoidina 1 , Metabolismo Energético , Humanos , Bromodesoxiuridina/metabolismo , Linhagem Celular Tumoral , Movimento Celular/fisiologia , Proliferação de Células/genética , Neoplasias Colorretais/genética , Neoplasias Colorretais/metabolismo , Diamida , Receptor com Domínio Discoidina 1/genética , Receptor com Domínio Discoidina 1/metabolismo , Receptores com Domínio Discoidina/metabolismo , Metabolismo Energético/genética , Ácido Láctico , Isoformas de Proteínas/metabolismo , Piruvato Quinase/metabolismo , Receptores Proteína Tirosina Quinases/metabolismo , Sincalida/metabolismo
11.
Ann Transl Med ; 9(18): 1429, 2021 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-34733981

RESUMO

BACKGROUND: Gut microbiome dysbiosis is related to the pathogenesis of nonalcoholic fatty liver disease (NAFLD), and the role of toll-like receptor 2 (TLR2) in its molecular mechanism is controversial. Here, we investigated the effects and mechanisms of Escherichia coli-derived lipopolysaccharide (LPS) on lipid accumulation and lipotoxicity in palmitic acid (PA)-treated L02 cell as an NAFLD cell model, and the role of TLR2 in this process. METHODS: Oil red O staining assay and free fatty acid (FFA) content test were performed to determine the effects of LPS on lipid accumulation in a PA-induced NAFLD cell model with or without TLR2 inhibition. The levels of IL-6 and TNF-α were measured to investigate inflammation conditions. Hoechst 33342 staining assay and Caspase-3 activity assay were used to test cell apoptosis, and the expression levels of proteins in the IRS1/PI3K/AKT signaling pathway, TLR2/MyD88/IKKα/NF-κB signaling pathway, and mitochondrion-dependent apoptotic signaling pathway were detected using Western blot. RESULTS: Lipid accumulation, pro-inflammatory cytokine release, and cell apoptosis with high levels were observed in the PA-induced NAFLD cell model, and LPS aggravated these processes. Whereas TLR2 inhibition could significantly ameliorate PA-induced and LPS-amplified lipid accumulation, inflammatory, and cell apoptosis, it had no significant effect on L02 cells treated with LPS alone. CONCLUSIONS: These results were confirmed by activation or inhibition of the IRS1/PI3K/AKT signaling pathway, TLR2/MyD88/IKKα/NF-κB signaling pathway, and mitochondrion-dependent apoptotic signaling pathway, and were reflected by changes on their proteins expression. TLR2 is involved in PA-induced lipid accumulation and lipotoxicity in L02 cells, which could be aggravated by LPS, although LPS-induced amplification might not be through direct interaction with TLR2.

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