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Synergistic effect of embossed Cu current collector and potassium nitrate for achieving dense lithium deposition and improving cycle life in anode-free Li metal batteries

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JOURNAL OF THE KOREAN CERAMIC SOCIETY 2024年第2期61卷 267-278页

作者： Ahn, Suhyun Song, Hyeonjun Kim, Sucheol Lee, Hojae Kim, Young-Beom Jang, Kihun Ha, Minsoo Ahn, Heejoon Hanyang Univ Dept Organ & Nano Engn 222 Wangsimni Ro Seoul 04763 South Korea Hanyang Univ Dept Battery Engn 222 Wangsimni Ro Seoul 04763 South Korea Hanyang Univ Dept Organ & Nano Engn Human Tech Convergence Program 222 Wangsimni Ro Seoul 04763 South Korea Hanyang Univ Dept Mech Engn 222 Wangsimni Ro Seoul 04763 South Korea Jeong Gwang Co LTD 861-41 Dongsan RiCheonbuk Myeon Gyeongju Si 86141 Gyeongsangbug D South Korea Hanyang Univ Inst Nano Sci & Technol 222 Wangsimni Ro Seoul 04763 South Korea

Anode-free lithium metal batteries (AFLMB) operate solely with lithium (Li) in the lithiated cathode, eliminating the mass and volume of the anode to maximize energy density of the battery. However, uneven Li deposition can lead to the formation of Li dendrites, hindering practical applications due to issues like solid electrolyte interphase (SEI) breakage and low coulombic efficiency (CE). To address these challenges, we investigated the synergistic effect of applying a 3D-structured current collector (CC) and KNO3 for Li deposition control. We fabricated an embossed Cu CC with a 3D structure using a copper nanoparticle (Cu NP) slurry and intense pulsed light (IPL) sintering techniques. When KNO3 electrolyte additives were used in conjunction with the manufactured 3D embossed Cu, we observed a significant improvement in cycle life. The KNO3 additive prevented the top plating of Li through an electrostatic shielding effect, while the anion contributed to dense Li deposition by forming a stable SEI layer, such as Li3N. Consequently, the combination of embossed Cu and KNO3 enabled thick and compact Li deposition, reducing Li loss during the plating and stripping processes and thereby improving the lifespan of the cell. In AFLMB matched with NCM811, capacity retention after 50 cycles increased to 52%, compared to 0.8% in the absence of electrolyte additives, demonstrating stable operation even after more than 100 cycles. Therefore, combining a thin, 3D-structured CC with an electrolyte additive capable of controlling Li deposition presents a promising strategy for enhancing the practical use of carbonate electrolyte-based AFLMB through synergistic effects.

关键词： Anode-free lithium metal batteries 3D structure current collector IPL sintering Electrostatic shielding

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Light-enhanced molecular polarity enabling multispectral color-cognitive memristor for neuromorphic visual system

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NATURE COMMUNICATIONS 2023年第1期14卷 5775页

作者： Lee, Jongmin Jeong, Bum Ho Kamaraj, Eswaran Kim, Dohyung Kim, Hakjun Park, Sanghyuk Park, Hui Joon Hanyang Univ Dept Organ & Nano Engn Seoul 04763 South Korea Hanyang Univ Human Tech Convergence Program Seoul 04763 South Korea Kongju Natl Univ Dept Chem Kong Ju 32588 South Korea Hanyang Inst Smart Semicond Seoul 04763 South Korea

An optoelectronic synapse having a multispectral color-discriminating ability is an essential prerequisite to emulate the human retina for realizing a neuromorphic visual system. Several studies based on the three-terminal transistor architecture have shown its feasibility;however, its implementation with a two-terminal memristor architecture, advantageous to achieving high integration density as a simple crossbar array for an ultra-high-resolution vision chip, remains a challenge. Furthermore, regardless of the architecture, it requires specific material combinations to exhibit the photo-synaptic functionalities, and thus its integration into various systems is limited. Here, we suggest an approach that can universally introduce a color-discriminating synaptic functionality into a two-terminal memristor irrespective of the kinds of switching medium. This is possible by simply introducing the molecular interlayer with long-lasting photo-enhanced dipoles that can adjust the resistance of the memristor at the light-irradiation. We also propose the molecular design principle that can afford this feature. The optoelectronic synapse array having a color-discriminating functionality is confirmed to improve the inference accuracy of the convolutional neural network for the colorful image recognition tasks through a visual pre-processing. Additionally, the wavelength-dependent optoelectronic synapse can also be leveraged in the design of a light-programmable reservoir computing system. Designing optoelectronic synapses having a multispectral color-discriminating ability is crucial for neuromorphic visual system. Here, the authors propose an strategy to introduce RGB color-discriminating synaptic functionality into a 2-terminals memristor regardless of switching medium and design a color image-recognizing CNN and light-programmable reservoir computing.

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Spontaneously Induced Hierarchical Structure by Surface Energy in Novel Conjugated Polymer-Based Ultrafast-Response Organic Photodetectors

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ADVANCED OPTICAL MATERIALS 2022年第9期10卷

作者： Jeong, WonJo Kang, Jinhyeon Lim, Soo Yeong Ahn, Hyungju Kim, Hyung Min Won, Jong Ho Jung, In Hwan Hanyang Univ Dept Organ & Nanoengn 222 Wangsimni Ro Seoul 04763 South Korea Hanyang Univ Human Tech Convergence Program 222 Wangsimni Ro Seoul 04763 South Korea Kookmin Univ Dept Chem 77 Jeongneung Ro Seoul 136702 South Korea POSTECH Pohang Accelerator Lab Pohang 37673 South Korea

A novel conjugated polymer, poly(4-(4,8-bis(5-(2-ethylhexyl)thiophen-2-yl)benzo[1,2-b:4,5-b']dithiophen-2-yl)-2,6-dioctylbenzo[1,2-d:4,5-d']bis(oxazole)) (PBB), is synthesized for use in ultrafast-response organic photodetectors (OPDs). The PBB synthesis is considered facile because a monomer could be isolated without column chromatography purification. The excellent solubility of PBB allows easy dissolution in both halogenated and nonhalogenated solvents, facilitating the fabrication of p-n heterojunction OPDs based-on PBB and 6,6-phenyl-C71-butyric acid methyl ester (PC71BM) using either chloroform (CF) or o-xylene (Xy). Notably, Xy-processed OPDs show superior performance with a responsivity (R) of 0.385 A W-1 and specific detectivity (D*) of 1.33 x 10(13) Jones at -1 V, whereas CF-based devices showed an R of 0.349 A W-1 and D* of 5.86 x 10(12) Jones. More importantly, Xy-processed OPDs exhibited an ultrafast signal response time of 3 mu s, which is much faster than that of CF-processed OPDs (42 mu s). These superior static and dynamic properties of PBB:PC71BM devices are achieved by the inverted hierarchical arrangement of PBB and PC71BM via a biased orientation of PC71BM toward the ZnO layer as well as a homogenous nanomorphology. This ideal morphology is spontaneously induced due to the difference in interfacial energy between PBB and PC71BM toward the ZnO surface and a well-mixed PBB:PC71BM blend in Xy solvent.

关键词： facile synthesis of conjugated polymer hierarchical arrangement high specific detectivity organic photodetector ultrafast response time

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Contribution of dark current density to the photodetecting properties of thieno[3,4-b]pyrazine-based low bandgap polymers

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DYES AND PIGMENTS 2022年 197卷 109910-109910页

作者： Kim, Hyeokjun Kang, Jinhyeon Ahn, Hyungju Jung, In Hwan Hanyang Univ Dept Organ & Nano Engn 222 Wangsimni Ro Seoul 04763 South Korea Hanyang Univ Human Tech Convergence Program 222 Wangsimni Ro Seoul 04763 South Korea Kookmin Univ Dept Chem 77 Jeongneung Ro Seoul 02707 South Korea POSTECH Pohang Accelerator Lab Pohang 37673 South Korea

Recently, near infrared (NIR) organic photodetectors (OPDs) have been extensively studied. Bulk heterojunction NIR OPDs composed of a high-bandgap polymer donor (PD) and a low-bandgap non-fullerene acceptor (NFA) showed the best performance, whereas the low-bandgap PD-based OPDs were relatively unsuccessful due to the high level of dark current density (Jd) under a negative bias. In this study, we synthesized three low-bandgap PDs based on a thieno[3,4-b]pyrazine (TP) moiety and developed red-NIR OPDs by blending them with a lowbandgap NFA. We found that the PD having a shallow HOMO energy level generated the largest ground-state electron transfer at negative bias, which overestimated the responsivity (R) and detectivity (D*) in OPDs. Notably, under weak light irradiation of 0.1 mW/cm2 at -2V, the contribution of Jd on Jph reached 99.6%. Thus, we modified the existing R and D* equations to better understand photodetecting properties at low light intensity, and these modified equations gave more realistic R and D* values in OPDs. On the other hand, a lowbandgap PD showing low Jd in OPDs was highly beneficial to detect a low light signal because the Jd negligibly contributed to Jph in OPDs. The low Jd values of OPDs at negative bias resulted in a high on/off signal ratio and constant R and D* values at different light intensities.

关键词： Red-NIR photodetectors Organic photodiodes Detectivity

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Sustainable 3D printing by reversible salting-out effects with aqueous salt solutions

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NATURE COMMUNICATIONS 2024年第1期15卷 1-12页

作者： Ji, Donghwan Liu, Joseph Zhao, Jiayu Li, Minghao Rho, Yumi Shin, Hwansoo Han, Tae Hee Bae, Jinhye Univ Calif San Diego Dept NanoEngn La Jolla CA 92093 USA Univ Calif San Diego Mat Sci & Engn Program La Jolla CA 92093 USA Univ Calif San Diego Chem Engn Program La Jolla CA 92093 USA Hanyang Univ Dept Organ & Nano Engn Seoul 04763 South Korea Hanyang Univ Human Tech Convergence Program Seoul 04763 South Korea

Achieving a simple yet sustainable printing technique with minimal instruments and energy remains challenging. Here, a facile and sustainable 3D printing technique is developed by utilizing a reversible salting-out effect. The salting-out effect induced by aqueous salt solutions lowers the phase transition temperature of poly(N-isopropylacrylamide) (PNIPAM) solutions to below 10 degrees C. It enables the spontaneous and instant formation of physical crosslinks within PNIPAM chains at room temperature, thus allowing the PNIPAM solution to solidify upon contact with a salt solution. The PNIPAM solutions are extrudable through needles and can immediately solidify by salt ions, preserving printed structures, without rheological modifiers, chemical crosslinkers, and additional post-processing steps/equipment. The reversible physical crosslinking and de-crosslinking of the polymer through the salting-out effect demonstrate the recyclability of the polymeric ink. This printing approach extends to various PNIPAM-based composite solutions incorporating functional materials or other polymers, which offers great potential for developing water-soluble disposable electronic circuits, carriers for delivering small materials, and smart actuators. Here, the authors show a facile and sustainable 3D printing by utilizing a reversible salting-out effect on poly(N-isopropylacrylamide) (PNIPAM) solutions. Aqueous salt solutions lower the phase transition temperature of PNIPAM solutions below 10 degrees C and instantly solidify the PNIPAM solutions upon contact.

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A printed highly stretchable supercapacitor by a combination of carbon ink and polymer network

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EXTREME MECHANICS LETTERS 2021年 49卷

作者： Song, Chiho Chen, Baohong Hwang, Jeonguk Lee, Sujin Suo, Zhigang Ahn, Heejoon Harvard Univ Kavli Inst Bionano Sci & Technol John A Paulson Sch Engn & Appl Sci Cambridge MA 02138 USA Hanyang Univ Dept Organ & Nano Engn Seoul 04763 South Korea Hanyang Univ Human Tech Convergence Program Seoul 04763 South Korea Hanyang Univ Inst Nano Sci & Technol Seoul 04763 South Korea

A supercapacitor requires two electronic conductors with large surface areas, separated by an ionic conductor. Here we demonstrate a method to print a highly stretchable supercapacitor. We formulate an ink by mixing graphene flakes and carbon nanotubes with an organic solvent, and use the ink to print two interdigitated electronic conductors on the surface of a dielectric elastomer. We then submerge the printed electronic conductors in an aqueous solution of monomer, photoinitiator, crosslinker, and salt. The organic solvent and water form a binary solvent in which the ions are mobile. Upon UV irradiation, a polymer network forms. In each printed electrode, the graphene flakes and carbon nanotubes form a percolating network, which interpenetrates the polymer network. The electronic and ionic conductors form large interfacial areas. When the supercapacitor is stretched, the graphene flakes and carbon nanotubes slide relative to one another, and the polymer network deforms by entropic elasticity. The polymer network traps individual graphene flakes and carbon nanotubes, so that repeated stretch neither breaks the percolating network nor shorts the two electrodes. The supercapacitor maintains 88% the initial capacitance after 1600 cycles of stretch to five times its initial dimension. The interpenetration of a covalent network of elastic polymer chains and a percolating network of conductive particles is generally applicable for making stretchable ionotronic devices. (C) 2021 Elsevier Ltd. All rights reserved.

关键词： Stretchable supercapacitors Printing Graphene Carbon nanotubes Stretchable ionotronic devices Polymer network

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Interfacial modification of wide-bandgap perovskite solar cell approaching 20% with organic hole transport material

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CHEMICAL ENGINEERING JOURNAL 2023年第1期474卷

作者： Heo, Jihyeon Lee, Seok Woo Yong, Jihye Park, Hansol Lee, Yu Kyung Shin, Juhwan Whang, Dong Ryeol Chang, Dong Wook Park, Hui Joon Hanyang Univ Dept Organ & Nano Engn Seoul 04763 South Korea Hanyang Univ Human Tech Convergence Program Seoul 04763 South Korea Hanyang Inst Smart Semicond Seoul 04763 South Korea Pukyong Natl Univ Dept Ind Chem Busan 48513 South Korea Hannam Univ Dept Adv Mat Daejeon 34054 South Korea

The interface modification of perovskite and charge transport is a key factor in improving the efficiency and stability of halide perovskite solar cells (PSCs). In particular, the characteristics of hole transport material (HTM) are crucial in inverted p-i-n structured devices, as they influence the perovskite crystallization and hole carrier extraction and transport. While NiOx is recognized as an efficient HTM due to its low cost, proper band gap, electrical conductivity, and high chemical stability, it has limitations such as rough morphology, poor surface quality, and low intrinsic conductivity. In this study, newly designed organic materials based on quinoxaline and triphenylamine that enhance the interfacial properties between NiOx and perovskite through passivation effect, reducing interface defect sites, are introduced to a wide-bandgap perovskite solar cell. We further confirm that the energy level alignment of these HTMs with the perovskite, along with their dipole moment, play a crucial role in enhancing the built-in potential of PSCs. Additionally, the hydrophobic characteristics of the HTMs improve the crystallinity of the perovskite layer. As a result, the performance and stability of the PSCs incorporating these HTMs are significantly enhanced, approaching high power conversion efficiency of 20%.

关键词： Perovksite solar cell Interface modification Organic hole transport material Nickel oxide

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Rational Design of Highly Soluble and Crystalline Conjugated Polymers for High-Performance Field-Effect Transistors

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ADVANCED ELECTRONIC MATERIALS 2022年第5期8卷

作者： Lee, Kyumin Jeong, Moon-Ki Suh, Eui Hyun Jeong, WonJo Oh, Jong Gyu Jang, Jaeyoung Jung, In Hwan Hanyang Univ Dept Energy Engn Seoul 04763 South Korea Seoul Natl Univ Sch Chem & Biol Engn 1 Gwanak Ro Seoul 08826 South Korea Hanyang Univ Dept Organ & Nano Engn 222 Wangsimni Ro Seoul 04763 South Korea Hanyang Univ Human Tech Convergence Program 222 Wangsimni Ro Seoul 04763 South Korea

Conjugated polymers based on cyclopentadithiophene (CPDT) moieties are widely used in optoelectronics applications but rarely in field-effect transistors (FETs). This is due to the steric hindrance at the tetrahedral center of the CPDT core, which is a critical problem requiring resolution without diminishing the polymer crystallinity and solubility. A bulky CPDT-based high-mobility copolymers are synthesized here, which shows excellent pi-pi stacking in the film states with good solubility. The addition of bulky ethylhexyl side chains to CPDT does not interfere with the molecular ordering and promotes the intercalation of linear alkyl chains on the co-monomeric units. The resulting polymer forms bimodal packing structures with strong lamellar ordering and pi-pi interactions. Furthermore, the free volume generated by the bulky ethylhexyl side chains allows for a small amount of fullerene additive to be contained in the film state without interfering with the molecular ordering, leading to enhanced on/off ratios and hole mobilities of the resulting FETs. As a result, promising hole mobilities of up to 1.08-1.64 cm(2) V-1 s(-1) are achieved with the optimized FETs, which are the highest mobilities reported for CPDT-based conjugated polymers containing branched alkyl side chains.

关键词： 3D charge transport pathway bulky branched alkyl side chains donor-acceptor conjugated polymers organic field-effect transistors side chain engineering

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Multimodal collective swimming of magnetically articulated modular nanocomposite robots

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NATURE COMMUNICATIONS 2022年第1期13卷 1-11页

作者： Won, Sukyoung Lee, Hee Eun Cho, Young Shik Yang, Kijun Park, Jeong Eun Yang, Seung Jae Wie, Jeong Jae Hanyang Univ Res Inst Ind Sci Seoul 04763 South Korea Inha Univ Program Environm & Polymer Engn Incheon 22212 South Korea SK Innovat Green Prod Solut Ctr Daejeon 34124 South Korea Seoul Natl Univ Dept Mat Sci & Engn Seoul 08826 South Korea Seoul Natl Univ Res Inst Adv Mat RIAM Seoul 08826 South Korea Inha Univ Educ & Res Ctr Smart Energy & Mat Dept Chem & Chem Engn Adv Nanohybrids Lab Incheon 22212 South Korea Hanyang Univ Dept Organ & Nano Engn Seoul 04763 South Korea Hanyang Univ Human Tech Convergence Program Seoul 04763 South Korea Hanyang Univ Dept Chem Engn Seoul 04763 South Korea Hanyang Univ Inst Nano Sci & Technol Seoul 04763 South Korea

Magnetically responsive composites can impart maneuverability to miniaturized robots. However, collective actuation of these composite robots has rarely been achieved, although conducting cooperative tasks is a promising strategy for accomplishing difficult missions with a single robot. Here, we report multimodal collective swimming of ternary-nanocomposite-based magnetic robots capable of on-demand switching between rectilinear translational swimming and rotational swimming. The nanocomposite robots comprise a stiff yet lightweight carbon nanotube yarn (CNTY) framework surrounded by a magnetic polymer composite, which mimics the hierarchical architecture of musculoskeletal systems, yielding magnetically articulated multiple robots with an agile above-water swimmability (similar to 180 body lengths per second) and modularity. The multiple robots with multimodal swimming facilitate the generation and regulation of vortices, enabling novel vortex-induced transportation of thousands of floating microparticles and heavy semi-submerged cargos. The controllable collective actuation of these biomimetic nanocomposite robots can lead to versatile robotic functions, including microplastic removal, microfluidic vortex control, and transportation of pharmaceuticals.

关键词： Carbon nanotubes and fullerenes Polymers

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A Review on the Applicability of Luminescent Phosphors and Effective Positioning in Dye-Sensitized Solar Cells for Enhanced Performance and Stability

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SOLAR RRL 2023年第22期7卷

作者： Muthu, Senthilkumar Gandhi, Mano Balaji Meenakshisundaram, Sai Prasanna Gandhi, Saravana Kumar Sridharan, Moorthy Babu Park, Hui Joon Hanyang Univ Dept Organ & Nano Engn Seoul 04763 South Korea Hanyang Univ Human Tech Convergence Program Seoul 04763 South Korea Anna Univ Crystal Growth Ctr Chennai 600025 Tamilnadu India Rajalakshmi Engn Coll Autonomous Dept Phys Chennai 602105 Tamilnadu India Hanyang Univ Hanyang Inst Smart Semicond Seoul 04763 South Korea

The narrow range of solar light absorption facilitated by the photoactive organic dyes has been restricting the significant development, and large-scale applications of dye-sensitized solar cells (DSSC). The major problem that limits the power conversion efficiency (PCE) of DSSC is the limitations of the organic dyes (light absorbers in DSSC) to absorb beyond the visible region of solar spectrum that resulting in lower PCE (& AP;13%) as compared with the commercialized technologies. Hence, the focus on developing efficient strategies to harvest the ultraviolet and infrared light regions of the solar spectrum and effective conversion into the absorption limit of dyes and thereby increasing the device performance and stability is the emerging technological development in DSSCs. Rare earth ion-doped upconversion (UC) and downconversion (DC) phosphors are the most promising solutions for the prevalent issues of the liquid junction solar cells. This review will focus on the emerging strategies for the PCE enhancement of DSSC with UC and DC materials. An exclusive review on the facile approach of simultaneous usage of both the UC and DC phosphors and the effective positioning of these spectral conversion phosphors, to achieve highly stable DSSCs with superior PCE is provided. A systematic summary of the applicability and multifunctional properties of spectral conversion phosphors on different regions of dye-sensitized solar cells (DSSCs) with suitable positioning, as well as the emerging trend of simultaneous usage of both the upconversion and downconversion phosphors in a single-junction DSSC architecture to realize the maximum possible efficiency and stability, is the main focus of this *** & COPY;2023 WILEY-VCH GmbH

关键词： downconversion dye-sensitized solar cells efficiency enhancement luminescent phosphors spectral conversion upconversion

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