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.
View Article and Find Full Text PDFCation exchange (CE) reaction is a classical synthesis method for creating complex structures. A lock of study on intrinsic mechanism limits its understanding and practical application. Using X-ray absorption spectroscopy, we observed that the evolution from Ru-Cl to Ru-O/OH occurs during the CE between KRuCl and CoSn(OH) in aqueous solution, while CE between KPtCl and CoSn(OH) is inhibited due to the failure of structural evolution from Pt-Cl to Pt-O/OH.
View Article and Find Full Text PDFCrystal-phase engineering that promotes the rearrangement of active atoms to form new structural frameworks achieves excellent result in the field of electrocatalysis and optimizes the performance of various electrochemical reactions. Herein, for the first time, it is found that the different components in metallic aerogels will affect the crystal-phase transformation, especially in high-entropy alloy aerogels (HEAAs), whose crystal-phase transformation during annealing is more difficult than medium-entropy alloy aerogels (MEAAs), but they still show better electrochemical performance. Specifically, PdPtCuCoNi HEAAs with the parent phase of face-centered cubic (FCC) PdCu possess excellent 89.
View Article and Find Full Text PDFAnion exchange membrane fuel cells are a potentially cost-effective energy conversion technology, however, the electrocatalyst for the anodic hydrogen oxidation reaction (HOR) suffers from sluggish kinetics under alkaline conditions. Herein, we report that Ru-based nanosheets with amorphous-crystalline heterointerfaces of Ru and Ti-doped RuO (a/c-Ru/Ti-RuO) can serve as a highly efficient HOR catalyst with a mass activity of 4.16 A mg, which is 19.
View Article and Find Full Text PDFExploring an active and cost-effective electrocatalyst alternative to carbon-supported platinum nanoparticles for alkaline hydrogen evolution reaction (HER) have remained elusive to date. Here, we report a catalyst based on platinum single atoms (SAs) doped into the hetero-interfaced Ru/RuO support (referred to as Pt-Ru/RuO), which features a low HER overpotential, an excellent stability and a distinctly enhanced cost-based activity compared to commercial Pt/C and Ru/C in 1 M KOH. Advanced physico-chemical characterizations disclose that the sluggish water dissociation is accelerated by RuO while Pt SAs and the metallic Ru facilitate the subsequent H* combination.
View Article and Find Full Text PDFBimetallic PtRu are promising electrocatalysts for hydrogen oxidation reaction in anion exchange membrane fuel cell, where the activity and stability are still unsatisfying. Here, PtRu nanowires were implanted with a series of oxophilic metal atoms (named as i-M-PR), significantly enhancing alkaline hydrogen oxidation reaction (HOR) activity and stability. With the dual doping of In and Zn atoms, the i-ZnIn-PR/C shows mass activity of 10.
View Article and Find Full Text PDFNoble metals have been widely used in catalysis, however, the scarcity and high cost of noble metal motivate researchers to balance the atomic efficiency and atomic density, which is formidably challenging. This article proposes a robust strategy for fabricating 3D amorphous noble metal-based oxides with simultaneous enhancement on atomic efficiency and density with the assistance of atomic channels, where the atomic utilization increases from 18.2% to 59.
View Article and Find Full Text PDFPhase regulation of noble metal-based nanomaterials provides a promising strategy for boosting the catalytic performance. However, realizing the continuous phase modulation in two-dimensional structures and unveiling the relevant structure-performance relationship remain significant challenges. In this work, we present the first example of continuous phase modulation in a library of Pd-Te hexagonal nanoplates (HNPs) from cubic-phase PdTe, rhombohedral-phase PdTe, rhombohedral-phase PdTe, and hexagonal-phase PdTe to hexagonal-phase PdTe.
View Article and Find Full Text PDFHO photosynthesis has attracted great interest in harvesting and converting solar energy to chemical energy. Nevertheless, the high-efficiency process of HO photosynthesis is driven by the low HO productivity due to the recombination of photogenerated electron-hole pairs, especially in the absence of a sacrificial agent. In this work, we demonstrate that ultrathin ZnInS nanosheets with S vacancies (S-ZIS) can serve as highly efficient catalysts for HO photosynthesis via O/HO redox.
View Article and Find Full Text PDFOxygen evolution reaction (OER) plays a key role in proton exchange membrane water electrolysis (PEMWE), yet the electrocatalysts still suffer from the disadvantages of low activity and poor stability in acidic conditions. Here, a new class of CdRu IrO nanoframes with distorted structure for acidic OER is successfully fabricated. Impressively, CdRu IrO displays an ultralow overpotential of 189 mV and an ultralong stability of 1500 h at 10 mA cm⁻ toward OER in 0.
View Article and Find Full Text PDFMariculture activities have been recognized as one of the major sources of contamination for marine pollutants, such as the excessive discharging of nitrogen and phosphate. The fully understanding of the pollutants emission and transportation is crucial for coastal environment management. However, the influence of such highly dynamic coastal process on the pollutant migration remain unclear, such as the effects of coastal seasonal hydrodynamics on the dissolved pollutant transportation, especially under intensive marine ranching activities in open waters.
View Article and Find Full Text PDFDesigning platinum (Pt)-based formic acid oxidation reaction (FAOR) catalysts with high performance and high selectivity of direct dehydrogenation pathway for direct formic acid fuel cell (DFAFC) is desirable yet challenging. Herein, we report a new class of surface-uneven PtPbBi/PtBi core/shell nanoplates (PtPbBi/PtBi NPs) as the highly active and selective FAOR catalysts, even in the complicated membrane electrode assembly (MEA) medium. They can achieve unprecedented specific and mass activities of 25.
View Article and Find Full Text PDFThickness regulation of transition metal hydroxides/oxides nanosheets with superior catalytic properties represents a promising strategy to enhance catalytic performance, but it remains an enormous challenge to achieve precise control, especially when it comes to the ultrathin limit (several atomic layers). In this work, a facile strategy of alkylamine-confined growth is proposed for the synthesis of thickness-tunable metal hydroxide/oxide nanosheets. Specifically, ultrathin cobalt hydroxide and cobaltous oxide hybrid (Co(OH)-CoO) nanosheets (Co-O NSs) with a thickness in the range of 2-6 nm (5-13 atomic layers) are synthesized by using alkylamines with different carbon chain lengths as the ligand to modulate vertical coordination ability.
View Article and Find Full Text PDFCatalytic reactions are surface-sensitive processes. Fabrication of homogeneous metastable metals can be used to promote phase-dependent catalytic performance; however, this has been a challenging task. Herein, homogeneous metastable hexagonal close-packed (hcp) Ir is epitaxially grown onto metastable phase hcp Ni, as demonstrated using spherical aberration electron microscopy.
View Article and Find Full Text PDFCarbon nanocages (CNCs) have attracted tremendous interest in heterogeneous catalysis due to their promising properties of porous structure and improved mass transfer. Nevertheless, the controlled synthesis of CNCs remains a great challenge. Herein, we have shown the successful construction of functionalized N-doped CNCs (NCNCs) via a one-stone-two-birds strategy.
View Article and Find Full Text PDFThe physicochemical properties and catalytic performance of transition metals are highly phase-dependent. Ru-based nanomaterials are superior catalysts toward hydrogen evolution reaction (HER) and hydrogen oxidation reaction (HOR), but studies are mostly limited to conventional hexagonal-close-packed (hcp) Ru, mainly arising from the difficulty in synthesizing Ru with pure face-centered-cubic (fcc) phase. Herein, we report a crystal-phase-dependent catalytic study of MoO-modified Ru (MoO-Ru fcc and MoO-Ru hcp) for bifunctional HER and HOR.
View Article and Find Full Text PDFRealizing stable and efficient overall water splitting is highly desirable for sustainable and efficient hydrogen production yet challenging because of the rapid deactivation of electrocatalysts during the acidic oxygen evolution process. Here, we report that the single-site Pt-doped RuO hollow nanospheres (SS Pt-RuO HNSs) with interstitial C can serve as highly active and stable electrocatalysts for overall water splitting in 0.5 M HSO.
View Article and Find Full Text PDFBreaking the bottleneck of hydrogen oxidation/evolution reactions (HOR/HER) in alkaline media is of tremendous importance for the development of anion exchange membrane fuel cells/water electrolyzers. Atomically dispersed active sites are known to exhibit excellent activity and selectivity toward diverse catalytic reactions. Here, a class of unique Rh Sb nanocrystals with multiple nanobranches (denoted as Rh Sb NBs) and atomically dispersed Rh sites are reported as promising electrocatalysts for alkaline HOR/HER.
View Article and Find Full Text PDFOver the past decades, despite the substantial efforts that have been devoted to the modifications of Pt nanoparticles (NPs) to tailor their selectivities for hydrogenation reactions, there are still a lack of facile strategies for precisely regulation of the surface properties of NPs, especially for those with small sizes. In this work, we propose a top-down thermal annealing strategy for tuning the surface properties of Pt-based NPs (≈4 nm) without the occurrence of aggregation. Compared to conventional bottom-up methods, the present top-down strategy can precisely regulate the surface compositions of Pt-Cd NPs and other ternary Pt-Cd-M NPs (M=Fe, Ni, Co, Mn, and Sn).
View Article and Find Full Text PDFHierarchical SnO₂ nanocrystallites aggregates (NAs) were prepared with a simple room temperature⁻based aqueous solution method followed by simple freeze-drying treatment. The as-prepared SnO₂ NAs were subsequently combined with SnO₂ nanosheet⁻based structures from the viewpoint of a function-matching strategy, and under an optimized condition, a power conversion efficiency (PCE) of 5.59% was obtained for the resultant hybrid photoanode, a remarkable 60% enhancement compared to that of dye-sensitized solar cells (DSCs) fabricated with bare SnO₂ NAs architecture.
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