Ruthenium (Ru)-based dual-site catalysts can efficiently accelerate alkaline hydrogen electrocatalytic kinetics by virtue of the well-balanced competitive adsorptions of multiple reaction intermediates. However, their insufficient mass transfer makes them far away from the applications, largely lying to the challenge of precisely manipulating the interface water structure. Herein, a concept of nitrogen-bridged positively charged dual sites with a robust interfacial hydrogen-bond network is presented for enhancing alkaline hydrogen oxidation and evolution reactions (HOR and HER).
View Article and Find Full Text PDFNat Commun
January 2025
Using metal oxides to disperse iridium (Ir) in the anode layer proves effective for lowering Ir loading in proton exchange membrane water electrolyzers (PEMWE). However, the reported low-Ir-based catalysts still suffer from unsatisfying electrolytic efficiency and durability under practical industrial working conditions, mainly due to insufficient catalytic activity and mass transport in the catalyst layer. Herein we report a class of porous heterogeneous nanosheet catalyst with abundant Ir-O-Mn bonds, achieving a notable mass activity of 4 A mg for oxygen evolution reaction at an overpotential of 300 mV, which is 150.
View Article and Find Full Text PDFAlloying has significantly upgraded the oxygen reduction reaction (ORR) of Pd-based catalysts through regulating the thermodynamics of oxygenated intermediates. However, the unsatisfactory activation ability of Pd-based alloys toward O molecules limits further improvement of ORR kinetics. Herein, the precise synthesis of nanosheet assemblies of spin-polarized PdCu-FeO in-plane heterostructures for drastically activating O molecules and boosting ORR kinetics is reported.
View Article and Find Full Text PDFJ Am Chem Soc
July 2024
An formed IrO ( ≤ 2) layer driven by anodic bias serves as the essential active site of Ir-based materials for oxygen evolution reaction (OER) electrocatalysis. Once being confined to atomic thickness, such an IrO layer possesses both a favorable ligand effect and maximized active Ir sites with a lower O-coordination number. However, limited by a poor understanding of surface reconstruction dynamics, obtaining atomic layers of IrO remains experimentally challenging.
View Article and Find Full Text PDFAlloying has proven power to upgrade metallic electrocatalysts, while the traditional alloys encounter limitation for optimizing electronic structures of surface metallic sites in a continuous manner. High-entropy alloys (HEAs) overcome this limitation by manageably tuning the adsorption/desorption energies of reaction intermediates. Recently, the marriage of nanotechnology and HEAs has made considerable progresses for renewable energy technologies, showing two important trends of size diminishment and multidimensionality.
View Article and Find Full Text PDFAdv Mater
August 2024
High-entropy alloys (HEAs) confine multifarious elements into the same lattice, leading to intense lattice distortion effect. The lattice distortion tends to induce local microstrain at atomic level and thus affect surface adsorptions toward different adsorbates in various electrocatalytic reactions, yet remains unexplored. Herein, this work reports a class of sub-2 nm IrRuRhMoW HEA nanoparticles (NPs) with distinct local microstrain induced by lattice distortion for boosting alkaline hydrogen oxidation (HOR) and evolution reactions (HER).
View Article and Find Full Text PDFJ Am Chem Soc
April 2024
The volumetric density of the metal atomic site is decisive to the operating efficiency of the photosynthetic nanoreactor, yet its rational design and synthesis remain a grand challenge. Herein, we report a shell-regulating approach to enhance the volumetric density of Co atomic sites onto/into multishell ZnCdS for greatly improving CO photoreduction activity. We first establish a quantitative relation between the number of shell layers, specific surface areas, and volumetric density of atomic sites on multishell ZnCdS and conclude a positive relation between photosynthetic performance and the number of shell layers.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2024
Electrocatalysis underpins the renewable electrochemical conversions for sustainability, which further replies on metallic nanocrystals as vital electrocatalysts. Intermetallic nanocrystals have been known to show distinct properties compared to their disordered counterparts, and been long explored for functional improvements. Tremendous progresses have been made in the past few years, with notable trend of more precise engineering down to an atomic level and the investigation transferring into more practical membrane electrode assembly (MEA), which motivates this timely review.
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October 2023
Ligand effect, induced by charge transfer between catalytic surface and substrate in core/shell structure, was widely proved to benefit Pt-catalyzed oxygen reduction reaction by tuning the position of d-band center of Pt theoretically. However, ligand effect is always convoluted by strain effect in real core/shell nanostructure; therefore, it remains experimentally unknown whether and how much the ligand effect solely contributes electrocatalytic activity improvements. Herein, we report precise synthesis of a kind of PdRu/Pt core/shell nanoplates with exclusive ligand effect for oxygen reduction reaction.
View Article and Find Full Text PDFAdvancing electrocatalysts for alkaline hydrogen oxidation/evolution reaction (HOR/HER) is essential for anion exchange membrane-based devices. The state-of-the-art Pt-based electrocatalysts for alkaline HOR suffer from low intrinsic activities and severe CO poisoning due to the challenge of simultaneously optimizing surface adsorption toward different adsorbates. Herein, this challenge is overcome by tuning an atomic MoO layer with high oxophilicity onto PtMo nanoparticles (NPs) with optimized H , OH , and CO adsorption for boosting anti-CO-poisoning hydrogen-cycle electrocatalysis in alkaline media.
View Article and Find Full Text PDFStudy Objective: Any abnormality of the uterine cavity can result in reduced endometrial receptivity, which negatively affects embryo implantation and leads to lower clinical pregnancy rates. The effects of improved uterine cavity environment on in vitro fertilization (IVF)/intracytoplasmic sperm injection (ICSI)-embryo transfer (ET) treatment outcome are unclear. This study aimed to investigate the impact of improved uterine cavity abnormalities on the pregnancy outcomes of infertile patients undergoing IVF/ICSI-ET.
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