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89 result(s) for "Liu, Yipu"
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Biaxial strain induced OH engineer for accelerating alkaline hydrogen evolution
The sluggish kinetics of Volmer step in the alkaline hydrogen evolution results in large energy consumption. The challenge that has yet well resolved is to control the water adsorption and dissociation. Here, we develop biaxially strained MoSe 2 three dimensional nanoshells that exhibit enhanced catalytic performance with a low overpotential of 58.2 mV at 10 mA cm −2 in base, and long-term stable activity in membrane-electrode-assembly based electrolyser at 1 A cm −2 . Compared to the flat and uniaxial-strained MoSe 2 , we establish that the stably adsorbed OH engineer on biaxially strained MoSe 2 changes the water adsorption configuration from O-down on Mo to O-horizontal on OH* via stronger hydrogen bonds. The favorable water dissociation on 3-coordinated Mo sites and hydrogen adsorption on 4-coordinated Mo sites constitute a tandem electrolysis, resulting in thermodynamically favorable hydrogen evolution. This work deepens our understanding to the impact of strain dimensions on water dissociation and inspires the design of nanostructured catalysts for accelerating the rate-determining step in multi-electron reactions. Hydroxide is the most abundant anion in alkaline solutions, but its impact on alkaline water electrolysis remains unclear. Herein, the authors report a biaxial strain induced OH engineer on MoSe 2 to accelerate alkaline hydrogen evolution by modifying the water dissociation.
Corrosion engineering towards efficient oxygen evolution electrodes with stable catalytic activity for over 6000 hours
Although a number of nonprecious materials can exhibit catalytic activity approaching (sometimes even outperforming) that of iridium oxide catalysts for the oxygen evolution reaction, their catalytic lifetimes rarely exceed more than several hundred hours under operating conditions. Here we develop an energy-efficient, cost-effective, scaled-up corrosion engineering method for transforming inexpensive iron substrates (e.g., iron plate and iron foam) into highly active and ultrastable electrodes for oxygen evolution reaction. This synthetic method is achieved via a desired corrosion reaction of iron substrates with oxygen in aqueous solutions containing divalent cations (e.g., nickel) at ambient temperature. This process results in the growth on iron substrates of thin film nanosheet arrays that consist of iron-containing layered double hydroxides, instead of rust. This inexpensive and simple manufacturing technique affords iron-substrate-derived electrodes possessing excellent catalytic activities and activity retention for over 6000 hours at 1000 mA cm -2 current densities. Earth-abundant water splitting materials are highly desirable for renewable fuel production, but such catalysts are rarely tested for long-term use. Here, the authors prepare active water-splitting electrocatalysts via corrosion engineering that are stable for thousands of hours.
Data-driven discovery of biaxially strained single atoms array for hydrogen production
The structure-performance relationship for single atom catalysts has remained unclear due to the averaged coordination information obtained from most single-atom catalysts. Periodic array of single atoms may provide a platform to tackle this inaccuracy. Here, we develop a data-driven approach by incorporating high-throughput density functional theory computations and machine learning to screen candidates based on a library of 1248 sites from single atoms array anchored on biaxial-strained transition metal dichalcogenides. Our screening results in Au atom anchored on biaxial-strained MoSe 2 surface via Au-Se 3 bonds. Machine learning analysis identifies four key structural features by classifying the ΔG H* data. We show that the average band center of the adsorption sites can be a predictor for hydrogen adsorption energy. This prediction is validated by experiments which show single-atom Au array anchored on biaxial-strained MoSe 2 archives 1000 hour-stability at 800 mA cm -2 towards acidic hydrogen evolution. Moreover, active hotspot consisting of Au atoms array and the neighboring Se atoms is unraveled for enhanced activity. The structure-performance relationship of single-atom catalysts remains unclear. Here a data-driven approach with high-throughput DFT and machine learning is used to screen 1248 single atoms arrays, to provide a better understanding of the hydrogen evolution reaction mechanism.
Reprogramming systemic and local immune function to empower immunotherapy against glioblastoma
The limited benefits of immunotherapy against glioblastoma (GBM) is closely related to the paucity of T cells in brain tumor bed. Both systemic and local immunosuppression contribute to the deficiency of tumor-infiltrating T cells. However, the current studies focus heavily on the local immunosuppressive tumor microenvironment but not on the co-existence of systemic immunosuppression. Here, we develop a nanostructure named Nano-reshaper to co-encapsulate lymphopenia alleviating agent cannabidiol and lymphocyte recruiting cytokine LIGHT. The results show that Nano-reshaper increases the number of systemic T cells and improves local T-cell recruitment condition, thus greatly increasing T-cell infiltration. When combined with immune checkpoint inhibitor, this therapeutic modality achieves 83.3% long-term survivors without recurrence in GBM models in male mice. Collectively, this work unveils that simultaneous reprogramming of systemic and local immune function is critical for T-cell based immunotherapy and provides a clinically translatable option for combating brain tumors. Glioblastoma (GBM) is characterized by local and systemic immunosuppression, showing limited responses to immunotherapies. Here the authors describe the design of a nanoplatform composed of the lymphopenia alleviating agent cannabidiol and the lymphocyte recruiting cytokine LIGHT, promoting anti-tumor immune responses in GBM preclinical models.
Systemic metastasis-targeted nanotherapeutic reinforces tumor surgical resection and chemotherapy
Failure of conventional clinical therapies such as tumor resection and chemotherapy are mainly due to the ineffective control of tumor metastasis. Metastasis consists of three steps: (i) tumor cells extravasate from the primary sites into the circulation system via epithelial-mesenchymal transition (EMT), (ii) the circulating tumor cells (CTCs) form “micro-thrombi” with platelets to evade the immune surveillance in circulation, and (iii) the CTCs colonize in the pre-metastatic niche. Here, we design a systemic metastasis-targeted nanotherapeutic (H@CaPP) composed of an anti-inflammatory agent, piceatannol, and an anti-thrombotic agent, low molecular weight heparin, to hinder the multiple steps of tumor metastasis. H@CaPP is found efficiently impeded EMT, inhibited the formation of “micro-thrombi”, and prevented the development of pre-metastatic niche. When combined with surgical resection or chemotherapy, H@CaPP efficiently inhibits tumor metastasis and prolonged overall survival of tumor-bearing mice. Collectively, we provide a simple and effective systemic metastasis-targeted nanotherapeutic for combating tumor metastasis. Failure of conventional clinical therapies such as tumor resection and chemotherapy are mainly due to the ineffective control of tumor metastasis. Here, the authors show that a systemic metastasis-targeted nanotherapeutic may offer a powerful adjunct therapy for suppressing tumor metastasis.
Substrate-adaptive sacrificial corrosion strategy enables 700 mV oxygen evolution window for enhanced seawater electrolysis
Seawater electrolysis for hydrogen production offers a sustainable solution to the energy crisis and freshwater scarcity. The presence of chloride ions triggers competitive chlorine oxidation at the anode, which rivals the oxygen evolution reaction and leads to pronounced reductions in overall efficiency and long-term stability. This challenge underscores the urgent need for highly efficient, durable, and scalable anode materials to accelerate the transition of seawater electrolysis from laboratory research to industrial application. In this work, we introduce a substrate-adaptive sacrificial corrosion strategy that enables the universal growth of highly active corrosion products on a wide range of conductive substrates, notably including stainless steel. The optimized electrode achieves an overpotential of 182 mV at 10 mA/cm 2 , and sustains 500 mA/cm 2 for 1000 h in 10  m KOH seawater. To fill the gap in describing anode selectivity, an oxygen evolution window is proposed and measured. The measured value of 700 mV, far exceeding the thermodynamic limit of 480 mV, provides compelling experimental evidence that kinetic regulation can break the thermodynamic framework. This work provides a scalable synthesis platform and mechanistic insights for designing industrial seawater electrolyzers with extended durability and selectivity. Seawater electrolysis for green hydrogen is hindered by corrosive chloride ions. Here, the authors report a substrate-adaptive sacrificial corrosion strategy for creating highly active anodes that resist seawater corrosion and break thermodynamic selectivity limits.
Metformin and histone deacetylase inhibitor based anti-inflammatory nanoplatform for epithelial-mesenchymal transition suppression and metastatic tumor treatment
Epithelial-mesenchymal transition (EMT), a differentiation process with aberrant changes of tumor cells, is identified as an initial and vital procedure for metastatic processes. Inflammation is a significant inducer of EMT and provides an indispensable target for blocking EMT, however, an anti-inflammatory therapeutic with highlighted safety and efficacy is deficient. Metformin is a promising anti-inflammatory agent with low side effects, but tumor monotherapy with an anti-inflammation drug could generate therapy resistance, cell adaptation or even promote tumor development. Combination therapies with various anti-inflammatory mechanisms can be favorable options improving therapeutic effects of metformin, here we develop a tumor targeting hybrid micelle based on metformin and a histone deacetylase inhibitor propofol-docosahexaenoic acid for efficient therapeutic efficacies of anti-inflammatory drugs. Triptolide is further encapsulated in hybrid micelles for orthotopic tumor therapies. The final multifunctional nanoplatforms (HAOPTs) with hyaluronic acid (HA) modification can target tumor efficiently, inhibit tumor cell EMT processes, repress metastasis establishment and suppress metastatic tumor development in a synergistic manner. Collectively, the results afford proof of concept that the tumor targeting anti-inflammatory nanoplatform can provide a potent, safe and clinical translational approach for EMT inhibition and metastatic tumor therapy.
Effectiveness of repeated low-level red light in myopia prevention and myopia control
Background/aimsTo compare the effects of repeated low-level red light (RLRL) treatment on axial length growth and refractive error changes in myopic and premyopic children.MethodsSubjects were assigned randomly to four subgroups: myopia-RLRL group (M-RL), myopia-control group (M-C), premyopia-RLRL group (PM-RL) and premyopia-control group (PM-C). Subjects in the RLRL group completed a 12-month treatment composed of a 3 min RLRL treatment session twice daily, with an interval of at least 4 hours, for 7 days per week. Visits were scheduled before and at 1-month, 3-month, 6-month, 9-month and 12-month follow-up after the treatment. Repeated-measures analysis of variance was used to compare the spherical equivalent refractive errors (SE) and axial length (AL) changes between the groups across the treatment period.ResultsAfter 12 months of treatment, in the myopia group, SE and AL changes were −0.078±0.375 D and 0.033±0.123 mm for M-RL and −0.861±0.556 D and 0.415±0.171 mm for M-C; in the premyopia group, the progression of SE and AL was −0.181±0.417 D and 0.145±0.175 mm for PM-RL and −0.521±0.436 D and 0.292±0.128 mm for PM-C. PM-RL indicated a lower myopia incidence than PM-C (2.5% vs 19.4%). Additionally, the percentage of AL shortening in the M-RL was higher than that in the PM-RL before the 9-month follow-up.ConclusionRLRL effectively delayed myopia progression in children with myopia and reduced the incidence of myopia in premyopic children. Moreover, RLRL exhibited a stronger impact on myopic children compared with premyopic individuals.
Growing Nanocrystalline Ru on Amorphous/Crystalline Heterostructure for Efficient and Durable Hydrogen Evolution Reaction
The design of efficient hydrogen evolution reaction (HER) catalysts to minimize reaction overpotentials plays a pivotal role in advancing water electrolysis and clean energy solutions. Ru-based catalysts, regarded as potential replacements for Pt-based catalysts, face stability challenges during catalytic process. The precise regulation of metal–support interactions effectively prevents Ru nanoparticle degradation while optimizing interfacial electronic properties, enabling the simultaneous enhancement of catalytic activity and stability. Herein, we design an amorphous/crystalline support and employ in situ replacement to develop a Ru-NiPx-Ni structure. The crystalline Ni phase with ordered atomic arrangement ensures efficient charge transport, while the amorphous phase with unsaturated dangling bonds provides abundant anchoring sites for Ru nanoclusters. This synergistic structure significantly enhances HER performance, which attains overpotentials of 19 mV at 10 mA cm−2 and 70 mV at 100 mA cm−2 in 1 m KOH, with sustained operation exceeding 55 h at 100 mA cm−2. Electrochemical impedance spectroscopy analysis confirms that the Ru-NiPx-Ni structure not only has a high density of active centers for HER, but also reduces the charge transfer resistance at the electrode–electrolyte interface, which effectively enhances HER kinetics. This study presents new directions for designing high-efficiency HER catalysts.
Engineering Amorphous CoNiRuOx Nanoparticles Grown on Nickel Foam for Boosted Electrocatalytic Hydrogen Evolution
Designing efficient and cost-effective electrocatalysts is crucial for the large-scale development of sustainable hydrogen energy. Amorphous catalysts hold great promise for application due to their structural flexibility and high exposure of active sites. We report a novel method for the in situ growth of amorphous CoNiRuOx nanoparticle structures (CoNiRuOx/NF) on a nickel foam substrate. In 1 m KOH, CoNiRuOx/NF achieves a current density of 10 mA/cm2 with a hydrogen evolution reaction (HER) overpotential of only 43 mV and remains stable for over 100 h at a current density of 100 mA/cm2. An alkaline electrolyzer assembled with CoNiRuOx/NF as the cathode delivers a current density 2.97 times higher than that of an IrO2||Pt/C electrode pair at the potential of 2 V and exhibits excellent long-term durability exceeding 100 h. Experimental results reveal that the combined replacement and corrosion reactions facilitate the formation of the amorphous CoNiRuOx structure. This work provides valuable insights for developing efficient and scalable amorphous catalysts.