Publications by authors named "Shixue Dou"

Current electrosynthesis catalysts typically rely on nanomaterial-based engineering with multi-dimensional structural modifications. However, such approaches may not always be necessary, especially for underexplored industrial electrochemical conversions. Here, we demonstrate that commercial platinum (Pt) foil catalysts excel in the electrochemical co-oxidation of waste polyethylene terephthalate (PET)-derived ethylene glycol (EG) and ammonia (NH) into formamide (HCONH), a process traditionally reliant on energy-intensive methods.

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Sodium metal batteries (SMBs) have emerged as promising candidates for next-generation energy storage systems, leveraging their high theoretical capacity and the natural abundance of Na resources. Nevertheless, critical challenges, including dendritic growth, side reactions, and pronounced volume fluctuations during cycling, continue to impede their commercialization. Conventional separators, including polyolefin or glass fiber types, suffer from poor wettability, uneven ion flux, and a rough surface.

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The tailorable confinement of high-entropy nanoparticles (HE-NPs) within molecular sieves (HE-NPs@MSs), synergizing merits of cocktail effects and geometric polymorphs, holds potential for advancing heterogeneous catalysis. However, effective and universal synthesis affording size homogeneity and production scalability remains elusive. In this contribution, we present a versatile strategy for encapsulating ultrafine HE-NPs within diverse mesoporous/microporous MSs to enable the rational construction of HE-NPs@MS library.

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The desolvation behavior of Li is widely regarded as primarily governed by the electrolyte composition, while the dynamic decoupling mechanism between the electrode interface and solvation structure has received limited attention. Herein, a competitive adsorption-driven, fast-ion-conducting host was innovatively developed based on the LiSi/LiN microrods. Guided by density functional theory (DFT) calculations and molecular dynamics (MD) simulations, it was revealed for the first time that the dual-phase interface exhibits competitive adsorption interactions with solvent molecules and anions within the solvation sheath.

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In recent years, research on lithium-ion and sodium-ion battery cathodes has advanced rapidly, with materials categorized into layered oxides, polyanionics, and Prussian blue analogues. Polyanionic cathodes stand out for sodium-ion batteries due to their structural stability, safety, and long cycle life, but face challenges in phase transition and property optimization. High-entropy doping has emerged as a key strategy to enhance their electrochemical performance.

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All-solid-state lithium-selenium batteries (ASSLSeBs) offer high energy density and improved safety for next-generation energy storage. Still, selenium cathodes suffer from large volume changes during cycling, leading to mechanical stress and rapid capacity fade. To address this, a stress-adaptive 2D graphene@Se composite cathode is developed, where small Se nanoparticles are anchored onto acid-treated expanded graphite (AcEG) to enhance charge transport and alleviate stress.

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Silicon (Si) has emerged as a prominent candidate for high-energy batteries due to its exceptionally high theoretical capacity and favorable lithiation potential. However, its electrochemical performance at subzero temperatures is significantly hampered by slow ion transport and sluggish ion diffusion processes. Here, we present a weakly solvating electrolyte formulated with 1 M lithium bis(fluorosulfonyl)imide (LiFSI) in a mixture of fluoroethylene carbonate (FEC) / methyl trifluoroacetate (MTFA).

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In contrast to high-concentration electrolyte systems, low-concentration electrolytes provide a cost-effective strategy to advance the commercialization of aqueous zinc-ion batteries (AZIBs). However, such electrolytes frequently exhibit severe dendrite formation caused by localized Zn concentration gradients, which critically compromise the cycling stability and operational safety of AZIBs. In this work, an innovative approach is proposed that involves the in situ construction of a fluoride-ion (F) enriched interfacial layer on zinc anodes.

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Prussian blue analogues (PBAs) are widely recognized as one of the most promising cathode materials for sodium-ion batteries (SIBs). However, many unqualified PBAs with unsatisfactory electrochemical performance are difficult to dispose of and pose a risk of environmental contamination. Additionally, the production process of layered oxides, another popular cathode material for SIBs, requires prolonged high-temperature sintering, resulting in significant energy consumption.

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Energy materials are essential for addressing global energy challenges, and their design, recycling, and performance optimization are critical for sustainable development. To efficiently rise to this occasion, advanced technology should be explored to address these challenges. This review focuses on the potential of ultrafast thermal engineering as an innovative approach to the design and recycling of energy materials and systematically examines ultrahigh temperature shock's origins, mechanisms, and developmental progress, clarifying fundamental differences between the Joule heating and carbothermal shock modes.

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Aqueous zinc-ion batteries (AZIBs) are gaining significant attention due to their excellent safety, cost-effectiveness, and environmental friendliness, making them highly competitive energy storage solutions. Despite these advantages, the commercial application of AZIBs faces substantial challenges, particularly those related to performance limitations of cathode materials. Among potential candidates, vanadium dioxide (VO) stands out due to its exceptional electrochemical properties and unique crystal structure, rendering it a promising cathode material for AZIB applications.

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Electrochemical conversion has been regarded as an ideal technology for achieving clean and sustainable energy, showing significant promise in addressing the increasingly serious energy crisis and environmental pollution. Ru-containing electrocatalysts (RUCE) outperform other precious metals due to elevated intrinsic activity and superior cost-effectiveness, developing into a promising candidate for electrochemical conversion reactions. A significant challenge in the field of catalyst discovery lies in its heavy reliance on empirical methods, rather than approaches that are rooted in rational design principles.

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As the latest representation of high-entropy materials, structurally ordered multi-component intermetallic (MCI) nanocrystals exhibit various attractive functional properties, exceptionally high activity, and durability in energy-related electrocatalytic applications. These properties are primarily attributed to their ordered superlattice structures and high-entropy effects in one sublattice. However, to date, MCI nanocrystals have not been systematically studied.

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The mechanisms underlying capacity fading during cycling in layered oxide cathode materials for sodium-ion batteries remain inadequately understood. It is essential to elucidate the reasons and propose effective strategies. Here, the capacity-fading mechanism of commercial NaFeMnNiO is due to the dissolution of iron ions.

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Azodicarbonamide (ADA) is selected as an additive to the polymer electrolyte (PE) to improve the stability of the NaFeMnNiO cathode. ADA can capture hydrogen from the polymer and induce local structures, enhancing the ionic conductivity of the PE. Moreover, the dehydrogenated ADA can bond to Fe ions, preventing the PE from decomposing.

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Zinc-ion secondary batteries have been competitive candidates since the "post-lithium-ion" era for grid-scale energy storage, owing to their plausible security, high theoretical capacity, plentiful resources, and environment friendliness. However, many encumbrances like notorious parasitic reactions and Zn dendrite growth hinder the development of zinc-ion secondary batteries remarkably. Faced with these challenges, eutectic electrolytes have aroused notable attention by virtue of feasible synthesis and high tunability.

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By modifying the coordination environment of single-Fe-atom active site, effective regulation of the photocatalytic oxygen reduction pathway can be achieved to attain high activity for photocatalytic oxidation of CH to CHOH in an aqueous solution. A comprehensive investigation is conducted to study the impact of different coordination numbers of single Fe atoms on photocatalytic CH oxidation reaction over carbon nitride. Among which, Fe/CN with a Fe-N3 coordination exhibit an exceptional photocatalytic performance in CH oxidation, reaching a remarkable methanol yield of 928.

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With the growing global demand for renewable energy and the increasing scarcity of lithium resources, sodium-ion batteries have received extensive attention and research as a potential alternative. Among many cathode materials for sodium-ion batteries, polyanion materials are favored for their high operating voltage, stable cycling performance, and good safety. However, the low electronic conductivity and low energy density of polyanionic materials limit their potential for large-scale commercial applications.

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Rechargeable zinc batteries (RZBs) are hindered by two primary challenges: instability of Zn anode and deterioration of the cathode structure in traditional aqueous electrolytes, largely attributable to the decomposition of active HO. Here, we design and synthesize a non-flammable water-in-dimethyl sulfoxide electrolyte to address these issues. X-ray absorption spectroscopy, in situ techniques and computational simulations demonstrate that the activity of HO in this electrolyte is extremely compressed, which not only suppresses the side reactions and increases the reversibility of Zn anode, but also diminishes the cathode dissolution and proton intercalation.

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Article Synopsis
  • The study explores heterojunction materials as effective electrocatalysts for enhancing lithium-sulfur (Li-S) battery performance.
  • It introduces a Bi2Te3/TiO2 topological insulator heterojunction that improves sulfur redox reaction kinetics by facilitating mass transport, capturing polysulfides, and speeding up their conversion.
  • The modified Li-S battery achieves impressive results with a specific capacity of 1375 mAh g-1, excellent cycling stability, and high performance even at elevated sulfur loadings.
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The adsorption-conversion paradigm of polysulfides during the sulfur reduction reaction (SRR) is appealing to tackle the shuttle effect in Li-S batteries, especially based upon atomically dispersed electrocatalysts. However, mechanistic insights into such catalytic systems remain ambiguous, limiting the understanding of sulfur electrochemistry and retarding the rational design of available catalysts. Herein, we systematically explore the polysulfide adsorption-conversion essence via a geminal-atom model system to understand the catalyst roles toward an expedited SRR.

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Recently, metal-based atomically thin materials (M-ATMs) have experienced rapid development due to their large specific surface areas, abundant electrochemically accessible sites, attractive surface chemistry, and strong in-plane chemical bonds. These characteristics make them highly desirable for energy-related conversion reactions. However, the insufficient active sites and slow reaction kinetics leading to unsatisfactory electrocatalytic performance limited their commercial application.

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Low-concentration electrolytes (LCEs) have attracted great attention due to their cost effectiveness and low viscosity, but suffer undesired organic-rich interfacial chemistry and poor oxidative stability. Herein, a unique latent solvent, 1,2-dibutoxyethane (DBE), is proposed to manipulate the anion-reinforced solvation sheath and construct a robust inorganic-rich interface in a 0.5 M electrolyte.

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Hydrogen peroxide (HO) electrosynthesis using metal-free carbon materials via the 2e oxygen reduction pathway has sparked considerable research interest. However, the scalable preparation of carbon electrocatalysts to achieve satisfactory HO yield in acidic media remains a grand challenge. Here, we present the design of a carbon nanoreactor series that integrates precise O/N codoping alongside well-regulated geometric structures targeting high-efficiency electrosynthesis of HO.

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