Showing papers by "Jun Lu published in 2021"

Halogenated Ti3C2 MXenes with Electrochemically Active Terminals for High-Performance Zinc Ion Batteries.

Abstract: The class of two-dimensional metal carbides and nitrides known as MXenes offer a distinct manner of property tailoring for a wide range of applications. The ability to tune the surface chemistry for expanding the property space of MXenes is thus an important topic, although experimental exploration of surface terminals remains a challenge. Here, we synthesized Ti3C2 MXene with unitary, binary, and ternary halogen terminals, e.g., -Cl, -Br, -I, -BrI, and -ClBrI, to investigate the effect of surface chemistry on the properties of MXenes. The electrochemical activity of Br and I elements results in the extraordinary electrochemical performance of the MXenes as cathodes for aqueous zinc ion batteries. The -Br- and -I-containing MXenes, e.g., Ti3C2Br2 and Ti3C2I2, exhibit distinct discharge platforms with considerable capacities of 97.6 and 135 mAh·g-1. Ti3C2(BrI) and Ti3C2(ClBrI) exhibit dual discharge platforms with capacities of 117.2 and 106.7 mAh·g-1. In contrast, the previously discovered MXenes Ti3C2Cl2 and Ti3C2(OF) exhibit no discharge platforms and only ∼50% of capacities and energy densities of Ti3C2Br2. These results emphasize the effectiveness of the Lewis-acidic-melt etching route for tuning the surface chemistry of MXenes and also show promise for expanding the MXene family toward various applications.

Atomic/molecular layer deposition for energy storage and conversion.

Abstract: Energy storage and conversion systems, including batteries, supercapacitors, fuel cells, solar cells, and photoelectrochemical water splitting, have played vital roles in the reduction of fossil fuel usage, addressing environmental issues and the development of electric vehicles. The fabrication and surface/interface engineering of electrode materials with refined structures are indispensable for achieving optimal performances for the different energy-related devices. Atomic layer deposition (ALD) and molecular layer deposition (MLD) techniques, the gas-phase thin film deposition processes with self-limiting and saturated surface reactions, have emerged as powerful techniques for surface and interface engineering in energy-related devices due to their exceptional capability of precise thickness control, excellent uniformity and conformity, tunable composition and relatively low deposition temperature. In the past few decades, ALD and MLD have been intensively studied for energy storage and conversion applications with remarkable progress. In this review, we give a comprehensive summary of the development and achievements of ALD and MLD and their applications for energy storage and conversion, including batteries, supercapacitors, fuel cells, solar cells, and photoelectrochemical water splitting. Moreover, the fundamental understanding of the mechanisms involved in different devices will be deeply reviewed. Furthermore, the large-scale potential of ALD and MLD techniques is discussed and predicted. Finally, we will provide insightful perspectives on future directions for new material design by ALD and MLD and untapped opportunities in energy storage and conversion.

1000 Wh L-1 lithium-ion batteries enabled by crosslink-shrunk tough carbon encapsulated silicon microparticle anodes.

Abstract: Microparticulate silicon (Si), normally shelled with carbons, features higher tap density and less interfacial side reactions compared to its nanosized counterpart, showing great potential to be applied as high-energy lithium-ion battery anodes. However, localized high stress generated during fabrication and particularly, under operating, could induce cracking of carbon shells and release pulverized nanoparticles, significantly deteriorating its electrochemical performance. Here we design a strong yet ductile carbon cage from an easily processing capillary shrinkage of graphene hydrogel followed by precise tailoring of inner voids. Such a structure, analog to the stable structure of plant cells, presents 'imperfection-tolerance' to volume variation of irregular Si microparticles, maintaining the electrode integrity over 1000 cycles with Coulombic efficiency over 99.5%. This design enables the use of a dense and thick (3 mAh cm-2) microparticulate Si anode with an ultra-high volumetric energy density of 1048 Wh L-1 achieved at pouch full-cell level coupled with a LiNi0.8Co0.1Mn0.1O2 cathode.

Intelligence-assisted predesign for the sustainable recycling of lithium-ion batteries and beyond

Abstract: The unprecedented consumption of lithium-ion batteries (LIBs) is occurring to meet the needs of modern transportation electrification. Recycling-friendly designs intrinsically facilitate the long-term sustainable utilization of natural resources, reducing the detrimental impacts of spent LIBs on the environment, and improving the economic viability of recycling. For this, we propose the incorporation of an intelligence-assisted predesign strategy into the battery-management system and battery chemistry, including ameliorating the traceability of battery structure and operation status, promoting cost-effective material sorting and separation, and adopting sustainable battery materials. The purposeful predesign of intelligent “Reuse–Refurbish–Recover” (3R) LIBs could be realized in an economically and environmentally sustainable (EES) manner. The intelligence-assisted predesign strategy will promote multi-disciplinary cooperation in a systematic and synergetic way; in addition, it will empower governments to establish and implement a series of regulations and standards for addressing the environmental pollution issues from spent batteries, thus avoiding the ever-increasing consumption of natural resources.

Prelithiated Li-Enriched Gradient Interphase toward Practical High-Energy NMC–Silicon Full Cell

Abstract: It is highly desirable to realize high-energy-density lithium-ion batteries consisting of nickel-rich layered oxide cathodes (Ni-rich NMC) and Si-based anodes. A critical challenge for Ni-rich NMC ...

5-Fluorouracil efficacy requires anti-tumor immunity triggered by cancer-cell-intrinsic STING.

Abstract: 5-Fluorouracil (5-FU) is a widely used chemotherapeutic drug, but the mechanisms underlying 5-FU efficacy in immunocompetent hosts in vivo remain largely elusive. Through modeling 5-FU response of murine colon and melanoma tumors, we report that effective reduction of tumor burden by 5-FU is dependent on anti-tumor immunity triggered by the activation of cancer-cell-intrinsic STING. While the loss of STING does not induce 5-FU resistance in vitro, effective 5-FU responsiveness in vivo requires cancer-cell-intrinsic cGAS, STING, and subsequent type I interferon (IFN) production, as well as IFN-sensing by bone-marrow-derived cells. In the absence of cancer-cell-intrinsic STING, a much higher dose of 5-FU is needed to reduce tumor burden. 5-FU treatment leads to increased intratumoral T cells, and T-cell depletion significantly reduces the efficacy of 5-FU in vivo. In human colorectal specimens, higher STING expression is associated with better survival and responsiveness to chemotherapy. Our results support a model in which 5-FU triggers cancer-cell-initiated anti-tumor immunity to reduce tumor burden, and our findings could be harnessed to improve therapeutic effectiveness and toxicity for colon and other cancers.

Exploring MXenes and their MAX phase precursors by electron microscopy

Abstract: This review celebrates the width and depth of electron microscopy methods and how these have enabled massive research efforts on MXenes. MXenes constitute a powerful recent addition to 2-dimensional materials, derived from their parent family of nanolaminated materials known as MAX phases. Owing to their rich chemistry, MXenes exhibit properties that have revolutionized ranges of applications, including energy storage, electromagnetic interference shielding, water filtering, sensors, and catalysis. Few other methods have been more essential in MXene research and development of corresponding applications, compared with electron microscopy, which enables structural and chemical identification at the atomic scale. In the following, the electron microscopy methods that have been applied to MXene and MAX phase precursor research are presented together with research examples and are discussed with respect to advantages and challenges.

Exosomal transfer of osteoclast-derived miRNAs to chondrocytes contributes to osteoarthritis progression

Abstract: Osteoarthritis (OA) is a prevalent aging-related joint disease lacking disease-modifying therapies. Here, we identified an upregulation of circulating exosomal osteoclast (OC)-derived microRNAs (OC-miRNAs) during the progression of surgery-induced OA in mice. We found that reducing OC-miRNAs by Cre-mediated excision of the key miRNA-processing enzyme Dicer or blocking the secretion of OC-originated exosomes by short interfering RNA-mediated silencing of Rab27a substantially delayed the progression of surgery-induced OA in mice. Mechanistically, the exosomal transfer of OC-miRNAs to chondrocytes reduced the resistance of cartilage to matrix degeneration, osteochondral angiogenesis and sensory innervation during OA progression by suppressing tissue inhibitor of metalloproteinase-2 (TIMP-2) and TIMP-3. Furthermore, systemic administration of a new OC-targeted exosome inhibitor (OCExoInhib) blunted the progression of surgery-induced OA in mice. We suggest that targeting the exosomal transfer of OC-miRNAs to chondrocytes represents a potential therapeutic avenue to tackle OA progression. The authors show that exosomal transfer of osteoclast-derived microRNAs to chondrocytes decreases the resistance of cartilage to matrix degeneration, angiogenesis and sensory innervation, and promotes osteoarthritis progression in mice.

Medial Parabrachial Nucleus Is Essential in Controlling Wakefulness in Rats.

Abstract: Activation of the parabrachial nucleus (PB) in the brainstem induced wakefulness in rats, suggesting which is an important nucleus that controls arousal. However, the sub-regions of PB in regulating sleep-wake cycle is still unclear. Here, we employ chemogenetics and optogenetics strategies and find that activation of the medial part of PB (MPB), but not the lateral part, induces continuous wakefulness for 10 h without sleep rebound in neither sleep amount nor the power spectra. Optogenetic activation of glutamatergic MPB neurons in sleeping rats immediately wake rats mediated by the basal forebrain (BF) and lateral hypothalamus (LH), but not the ventral medial thalamus. Most importantly, chemogenetic inhibition of PB neurons decreases wakefulness for 10 h. Conclusively, these findings indicate that the glutamatergic MPB neurons are essential in controlling wakefulness, and that MPB-BF and MPB-LH pathways are the major neuronal circuits.

Fabrication and properties of Cf/(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C-SiC high-entropy ceramic matrix composites via precursor infiltration and pyrolysis

Abstract: In this work, Cf/(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C-SiC high-entropy ceramic matrix composites were reported for the first time. Based on the systematic study of the pyrolysis and solid-solution mechanisms of (Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C precursor by Fourier transform infrared spectroscopy, TG-MS and XRD, Cf/(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C-SiC with uniform phase and element distribution were successfully fabricated by precursor infiltration and pyrolysis. The as-fabricated composites have a density and open porosity of 2.40 g/cm3 and 13.32 vol% respectively, with outstanding bending strength (322 MPa) and fracture toughness (8.24 MPa m1/2). The Cf/(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C-SiC composites also present excellent ablation resistant property at a heat flux density of 5 MW/m2, with linear and mass recession rates of 2.89 μm/s and 2.60 mg/s respectively. The excellent combinations of mechanical and ablation resistant properties make the Cf/(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C-SiC composites a new generation of reliable ultra-high temperature materials.

Energy-constrained Self-training for Unsupervised Domain Adaptation

Abstract: Unsupervised domain adaptation (UDA) aims to transfer the knowledge on a labeled source domain distribution to perform well on an unlabeled target domain. Recently, the deep self-training involves an iterative process of predicting on the target domain and then taking the confident predictions as hard pseudo-labels for retraining. However, the pseudo-labels are usually unreliable, and easily leading to deviated solutions with propagated errors. In this paper, we resort to the energy-based model and constrain the training of the unlabeled target sample with the energy function minimization objective. It can be applied as a simple additional regularization. In this framework, it is possible to gain the benefits of the energy-based model, while retaining strong discriminative performance following a plug-and-play fashion. We deliver extensive experiments on the most popular and large scale UDA benchmarks of image classification as well as semantic segmentation to demonstrate its generality and effectiveness.

Identity-aware Facial Expression Recognition in Compressed Video

Abstract: This paper targets to explore the inter-subject variations eliminated facial expression representation in the compressed video domain. Most of the previous methods process the RGB images of a sequence, while the off-the-shelf and valuable expression-related muscle movement already embedded in the compression format. In the up to two orders of magnitude compressed domain, we can explicitly infer the expression from the residual frames and possible to extract identity factors from the I frame with a pre-trained face recognition network. By enforcing the marginal independent of them, the expression feature is expected to be purer for the expression and be robust to identity shifts. We do not need the identity label or multiple expression samples from the same person for identity elimination. Moreover, when the apex frame is annotated in the dataset, the complementary constraint can be further added to regularize the feature-level game. In testing, only the compressed residual frames are required to achieve expression prediction. Our solution can achieve comparable or better performance than the recent decoded image based methods on the typical FER benchmarks with about 3× faster inference with compressed data.

Molecular Classification of Knee Osteoarthritis.

Abstract: Knee osteoarthritis (KOA) is the most common form of joint degeneration with increasing prevalence and incidence in recent decades. KOA is a molecular disorder characterized by the interplay of numerous molecules, a considerable number of which can be detected in body fluids, including synovial fluid, urine, and blood. However, the current diagnosis and treatment of KOA mainly rely on clinical and imaging manifestations, neglecting its molecular pathophysiology. The mismatch between participants' molecular characteristics and drug therapeutic mechanisms might explain the failure of some disease-modifying drugs in clinical trials. Hence, according to the temporal alteration of representative molecules, we propose a novel molecular classification of KOA divided into pre-KOA, early KOA, progressive KOA, and end-stage KOA. Then, progressive KOA is furtherly divided into four subtypes as cartilage degradation-driven, bone remodeling-driven, inflammation-driven, and pain-driven subtype, based on the major pathophysiology in patient clusters. Multiple clinical findings of representatively investigated molecules in recent years will be reviewed and categorized. This molecular classification allows for the prediction of high-risk KOA individuals, the diagnosis of early KOA patients, the assessment of therapeutic efficacy, and in particular, the selection of homogenous patients who may benefit most from the appropriate therapeutic agents.

Proteins extracted from seaweed Undaria pinnatifida and their potential uses as foods and nutraceuticals.

Abstract: Isolation and utilization of proteins from seaweeds have been a novel trend in the world at present due to the increasing demand for healthy non-animal proteins. The attention of scientific community has been paid on the protein derived from seaweed Undaria pinnatifida due to their high nutritional quality and bioactivity. This article aims to provide an integrated overview on methods of extraction, isolation and purification of U. pinnatifida-derived proteins and composition, nutritional value and potential nutraceutical and food applications with an interest to stimulate further research to optimize the utilization. Potential food applications of U. pinnatifida derived proteins are nutritional components in human diet, food ingredients and additives, alternative meat and meat analogues and animal and fish feed. Excellent antioxidant, antihypertension, anticoagulant, anti-diabetes, antimicrobial and anti-cancer activities possessed by proteins of U. pinnatifida enable the use of these proteins in various nutraceutical applications. A number of studies have been carried out on antioxidant and antihypertensive activities of U. pinnatifida proteins, whereas other bioactivites are yet to be further studied. Hence, more research works are crucial to be done in order to facilitate and promote the emerging novel foods and nutraceuticals, using proteins from seaweed U. pinnatifida.

Electrochemical Lithium Storage Performance of Molten Salt Derived V2SnC MAX Phase.

Abstract: MAX phases are gaining attention as precursors of two-dimensional MXenes that are intensively pursued in applications for electrochemical energy storage. Here, we report the preparation of V2SnC MAX phase by the molten salt method. V2SnC is investigated as a lithium storage anode, showing a high gravimetric capacity of 490 mAh g−1 and volumetric capacity of 570 mAh cm−3 as well as superior rate performance of 95 mAh g−1 (110 mAh cm−3) at 50 C, surpassing the ever-reported performance of MAX phase anodes. Supported by operando X-ray diffraction and density functional theory, a charge storage mechanism with dual redox reaction is proposed with a Sn–Li (de)alloying reaction that occurs at the edge sites of V2SnC particles where Sn atoms are exposed to the electrolyte followed by a redox reaction that occurs at V2C layers with Li. This study offers promise of using MAX phases with M-site and A-site elements that are redox active as high-rate lithium storage materials.

Fabrication and optimization of 3D-Cf/HfC-SiC-based composites via sol-gel processing and reactive melt infiltration

Abstract: In this work, 3D-Cf/HfC-SiC-based composites were fabricated and optimized via reactive melt infiltration (RMI) of Si into porous Cf/HfC-C preforms prepared by a sol-gel processing. The physical and chemical processes involved during the fabrication were identified and analyzed in details. It is revealed that fibers and interphase of the composites can be eroded during carbothermal reduction process, which can be further aggravated during RMI, with the formation of Hf-containing substance on the fibers surface. The fibers and interphase degradation is mainly induced by the reactions between HfO2 and C/SiC interphase layers at elevated temperatures. Accordingly, a two-step carbothermal reduction treatment was proposed for the optimization of the fabrication procedure. As a result, less fiber/interphase erosion and improved mechanical properties are achieved in the composites, with the bending strength increased by ∼49 % (from 214.1 ± 15.7 MPa to 319.0 ± 26.0 MPa).

Lessons Learned From the Prototypes of the MQXFA Low-Beta Quadrupoles for HL-LHC and Status of Production in the US

Abstract: With the successful test of the first two pre-series magnets the US HL-LHC Accelerator Upgrade Project has started production of the MQXFA magnets to be used in Q1/Q3 inner triplet elements of the HL-LHC. This good start comes after the test of two prototypes with limited performance, and it demonstrates the importance of learning from past issues. Therefore, in this paper we want to share the most important lessons learned so far, focusing on those which may be more interesting for similar projects. We will also present the status of MQXFA fabrication in the US.