Publications by authors named "Pao C"

Methanol (ME) is a liquid hydrogen carrier, ideal for on-site-on-demand H generation, avoiding its costly and risky distribution issues, but this "ME-to-H" electric conversion suffers from high voltage (energy consumption) and competitive oxygen evolution reaction. Herein, we demonstrate that a synergistic cofunctional PtPd/(Ni,Co)(OH) catalyst with Pt single atoms (Pt) and Pd nanoclusters (Pd) anchored on OH-vacancy(V)-rich (Ni,Co)(OH) nanoparticles create synergistic triadic active sites, allowing for methanol-enhanced low-voltage H generation. For MOR, OH* is preferentially adsorbed on Pd and then interacts with the intermediates (such as *CHO or *CHOOH) adsorbed favorably on neighboring Pt with the assistance of hydrogen bonding from the surface hydrogen of (Ni,Co)(OH).

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CaCuFeReO and LaCuFeReO quadruple perovskite oxides are well known for their high ferrimagnetic Curie temperatures and half-metallic electronic structures. By A-site chemical substitution with lower valence state Na, an isostructural compound NaCuFeReO with both A- and B-site ordered quadruple perovskite structures in -3 symmetry was prepared using high-pressure and high-temperature techniques. The X-ray absorption study demonstrates the valence states to be Cu, Fe, and Re.

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Oxygen and water generating hydrogen peroxide (HO) by optical drive is an extremely promising pathway, and the large amount of oxygen in air and natural sunlight illumination are excellent catalytic conditions. However, the separation efficiency of photogenerated electron-hole pairs greatly limits the photocatalytic efficiency, especially in the absence of sacrificial agents. Here, we report an InS nanosheet with an S vacancy (S-InS).

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PtRu-based catalysts toward hydrogen oxidation reaction (HOR) suffer from low efficiency, CO poisoning and over-oxidation at high potentials. In this work, an amorphization strategy is adopted for preparation of amorphous SrRuPtOH nanobelts (a-SrRuPtOH NBs). The a-SrRuPtOH NBs has optimized adsorption of intermediates (H and OH), increased number of active sites, highly weakened CO poisoning and enhanced anti-oxidation ability owing to the special amorphous structure.

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Article Synopsis
  • Tetrahedral, pyramidal, and octahedral metal-oxygen coordinated ligands are key to metal-oxide structures, with their behavior during electrochemical oxidation being critical yet underexplored.
  • A study links oxygen-evolving performance to structural properties of model oxides, finding that pyramidal structures are more vulnerable to hydroxide (OH) attacks, leading to transformation into active amorphous CoOOH.
  • The research proposes an ion-tuning strategy to improve both activity and stability in metal oxides, addressing the challenge of balancing performance and structural durability in electrochemical applications.
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Methane (CH) photocatalytic upgrading to value-added chemicals, especially C products, is significant yet challenging due to sluggish energy/mass transfer and insufficient chemical driven-force in single photochemical process. Herein, we realize solar-driven CH oxidation to ethanol (CHOH) on crystalline carbon nitride (CCN) modified with CuS and Cu single atoms (CuS/Cu-CCN). The integration of photothermal effect and photocatalysis overcomes CH-to-CHOH conversion bottlenecks, with CuS as a hotspot to convert solar-energy to heat.

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As one of the best candidates for hydrogen oxidation reaction (HOR), ruthenium (Ru) has attracted significant attention for anion exchange membrane fuel cells (AEMFCs), although it suffers from sluggish kinetics under alkaline conditions due to its strong hydroxide affinity. In this work, we develop ternary hollow nanocages with Pt epitaxy on RuCu (Pt-RuCu NCs) as efficient HOR catalysts for application in AEMFCs. Experimental characterizations and theoretical calculations confirm that the synergy in optimized Pt-RuCu NCs significantly modifies the electronic structure and coordination environment of Ru, thereby balancing the binding strengths of H* and OH* species, which leads to a markedly enhanced HOR performance.

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Proton exchange membrane water electrolyzers powered by sustainable energy represent a cutting-edge technology for renewable hydrogen generation, while slow anodic oxygen evolution reaction (OER) kinetics still remains a formidable obstacle that necessitates basic comprehension for facilitating electrocatalysts' design. Here, we report a low-iridium complex oxide LaSrIrO with a unique hexagonal structure consisting of isolated Ir(V)O octahedra and true peroxide O groups as a highly active and stable OER electrocatalyst under acidic conditions. Remarkably, LaSrIrO, containing 59 wt % less iridium relative to the benchmark IrO, shows about an order of magnitude higher mass activity, 6-folds higher intrinsic activity than the latter, and also surpasses the state-of-the-art Ir-based oxides ever reported.

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Accelerating the alkaline hydrogen evolution reaction (HER), which involves the slow cleavage of HO-H bonds and the adsorption/desorption of hydrogen (H*) and hydroxyl (OH*) intermediates, requires developing catalysts with optimal binding strengths for these intermediates. Here, the unconventional hexagonal close-packed (HCP) high-entropy alloy (HEA) atomic layers are prepared composed of five platinum-group metals to enhance the alkaline HER synergistically. The breakthrough is made by layer-by-layer heteroepitaxial deposition of subnanometer RuRhPdPtIr HEA layers on the HCP Ru seeds, despite the thermodynamic stability of Rh, Pd, Pt, and Ir in a face-centered cubic (FCC) structure except for Ru.

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High-entropy perovskite oxides exhibit promising application prospects in the field of electrocatalysis, owing to their flexible elemental composition, plentiful active sites, and superior structural stability. Herein, high-entropy perovskite oxide nanotubes are prepared with La, Nd, Pr, Er, Eu at A-site by electrospinning as efficient electrocatalysts for nitrate reduction reaction (NORR). Electrochemical tests demonstrate that LaNdPrErEuCuO nanotubes (LNPEEC NTs) display outstanding NORR performance, achieving a NH Faraday efficiency (FE) of 100% at -0.

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Developing efficient electrocatalysts for acidic electrosynthesis of hydrogen peroxide (HO) holds considerable significance, while the selectivity and stability of most materials are compromised under acidic conditions. Herein, we demonstrate that constructing amorphous platinum-selenium (Pt-Se) shells on crystalline Pt cores can manipulate the oxygen reduction reaction (ORR) pathway to efficiently catalyze the electrosynthesis of HO in acids. The Se‒Pt nanoparticles, with optimized shell thickness, exhibit over 95% selectivity for HO production, while suppressing its decomposition.

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Article Synopsis
  • Cation exchange (CE) is a key method for synthesizing complex structures, but understanding its intrinsic mechanisms has been limited.
  • X-ray absorption spectroscopy revealed that during CE, Ru transitions from Ru-Cl to Ru-O/OH, while Pt does not undergo this change, affecting its reactivity with CoSn(OH).
  • The study shows that the electron transfer interaction with Co vacancy enhances CE performance, leading to the development of highly efficient, Pt-free CoRuSn(OH) catalysts with superior activity and power density compared to commercial PtRu/C, paving the way for advancements in fuel cell technology.
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Pt-based nanoparticles (NPs) have been widely used in catalysis. However, this suffers from aggregation and/or sintering at working conditions. We demonstrate a robust strategy for stabilizing PtCo NPs under high temperature with strong interaction between M-N-C and PtCo NPs with Pt-M-N coordination, namely, "atom glue.

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While luminescent stimuli-responsive materials (LSRMs) have become one of the most sought-after materials owing to their potential in optoelectronic applications, the use of earth-scarce lanthanides remains a crucial problem to be solved for further development. In this work, two manganese-based LSRMs, ()-(+)-1-phenylethylammonium manganese bromide, (R-PEA)MnBr, and ()-(-)-1-phenylethylammonium manganese bromide, (S-PEA)MnBr, are successfully demonstrated. Both (R-PEA)MnBr and (S-PEA)MnBr show a kinetically stable red-emissive amorphous state and a thermodynamically stable green-emissive crystalline state at room temperature, where the fully reversible transition can be done through melt-quenching and annealing processes.

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Rechargeable zinc-air batteries (ZABs) are viewed as a promising solution for electric vehicles due to their potential to provide a clean, cost-effective, and sustainable energy storage system for the next generation. Nevertheless, sluggish kinetics of the oxygen evolution reaction (OER), the oxygen reduction reaction (ORR) at the air electrode, and low power density are significant challenges that hinder the practical application of ZABs. The key to resolving the development of ZABs is developing an affordable, efficient, and stable catalyst with bifunctional catalytic.

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An efficient and facile water dissociation process plays a crucial role in enhancing the activity of alkaline hydrogen evolution reaction (HER). Considering the intricate influence between interfacial water and intermediates in typical catalytic systems, meticulously engineered catalysts should be developed by modulating electron configurations and optimizing surface chemical bonds. Here, a high-entropy double perovskite (HEDP) electrocatalyst La(CoNiMgZnNaLi)RuO, achieving a reduced overpotential of 40.

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Identifying new molecular therapies targeted at the severe hepatic fibrosis associated with the granulomatous immune response to Schistosoma mansoni infection is essential to reduce fibrosis-related morbidity/mortality in schistosomiasis. In vitro cell activation studies suggested the lipid molecule prostaglandin D2 (PGD2) as a potential pro-fibrotic candidate in schistosomal context, although corroboratory in vivo evidence is still lacking. Here, to investigate the role of PGD2 and its cognate receptor DP2 in vivo, impairment of PGD2 synthesis by HQL-79 (an inhibitor of the H-PGD synthase) or DP2 receptor inhibition by CAY10471 (a selective DP2 antagonist) were used against the fibrotic response of hepatic eosinophilic granulomas of S.

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The insufficient availability and activity of interfacial water remain a major challenge for alkaline hydrogen evolution reaction (HER). Here, we propose an "on-site disruption and near-site compensation" strategy to reform the interfacial water hydrogen bonding network via deliberate cation penetration and catalyst support engineering. This concept is validated using tip-like bimetallic RuNi nanoalloys planted on super-hydrophilic and high-curvature carbon nanocages (RuNi/NC).

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Proton exchange membrane water electrolysers promise to usher in a new era of clean energy, but they remain a formidable obstacle in designing active and durable electrocatalysts for the acidic oxygen evolution reaction (OER). In this study, a protonated iridium oxide embedded with single-atom dispersed ruthenium atoms (HIr RuO) that demonstrates exceptional activity and stability in acidic water oxidation is introduced. The single Ru dopants favorably induce localized oxygen vacancies in the Ir─O lattice, synergistically strengthening the adsorption of OOH* intermediates and enhancing the intrinsic OER activity.

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This study emphasizes the innovative application of FePt and Cu core-shell nanostructures with increased lattice microstrain, coupled with Au single-atom catalysis, in significantly enhancing OH generation for catalytic tumor therapy. The combination of core-shell with increased lattice microstrain and single-atom structures introduces an unexpected boost in hydroxyl radical (OH) production, representing a pivotal advancement in strategies for enhancing reactive oxygen species. The creation of a core-shell structure, FePt@Cu, showcases a synergistic effect in OH generation that surpasses the combined effects of FePt and Cu individually.

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Intermetallic alloys have traditionally been characterized by their inherent brittleness due to their lack of sufficient slip systems and absence of strain hardening. However, here we developed a single-phase B2 high-entropy intermetallic alloy that is both strong and plastic. Unlike conventional intermetallics, this high-entropy alloy features a highly distorted crystalline lattice with complex chemical order, leading to multiple slip systems and high flow stress.

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High-entropy perovskite oxides are promising materials in the field of electrocatalysis due to their advantages such as large spatial composition regulation, entropy effects, and tunable material properties. However, the preparation of high-entropy perovskite oxides with stable and controllable structures still remains challenging. Herein, we fabricated a series of high-entropy perovskite oxide porous nanotubes (PNTs) by electrospinning as efficient electrocatalysts for the nitrate reduction reaction (NORR).

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We report a catalyst family of high-entropy alloy (HEA) atomic layers having three elements from iron-group metals (IGMs) and two elements from platinum-group metals (PGMs). Ten distinct quinary compositions of IGM-PGM-HEA with precisely controlled square atomic arrangements are used to explore their impact on hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR). The PtRuFeCoNi atomic layers perform enhanced catalytic activity and durability toward HER and HOR when benchmarked against the other IGM-PGM-HEA and commercial Pt/C catalysts.

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A strain engineering strategy is crucial for designing a high-performance catalyst. However, how to control the strain in metastable phase two-dimensional (2D) materials is technically challenging due to their nanoscale sizes. Here, we report that cerium dioxide (CeO) is an ideal loading material for tuning the in-plane strain in 2D metastable 1T-phase IrO (1T-IrO) via an in situ growth method.

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Purpose: Diet plays a fundamental role in promoting resilience against stress-related disorders. We aimed to examine the overall and sex-specific association between food groups and perceived stress in adults.

Methods: We analyzed the prospective data of 7,434 adults who completed both the 2011 and 2015 surveys of the China Health and Nutrition Survey (CHNS).

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