Developing innovative resource utilization strategies to achieve sustainable recycling of waste-to-fuel is highly desirable, yet the design of cost-effective bifunctional catalysts with dual high-efficiency remains unexplored. While the Fenton-like reaction relies on enhancing peroxymonosulfate (PMS) adsorption and accelerating interfacial electron transfer to improve kinetic rates, CO reduction is constrained by sluggish kinetics and competing hydrogen evolution reaction. Herein, we construct a bifunctional catalyst (NiFe-BNC) featuring dual-atomic active sites by introducing boron atoms into a biomass-derived chitosan substrate rich in functional groups, which optimizes atomic coordination environments.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2025
Electrocatalytic acetylene semihydrogenation in membrane electrode assembly systems promises a sustainable pathway for ethylene production, yet faces challenges in catalyst performance and durability. Herein, we developed a Cu coordination polymer with hybrid sites that synergistically integrate open Cu sites and N-heterocyclic carbenes. These hybrid sites bestow the coordination polymer with acetylene gasophilicity, hydrophobicity toward water, and readily accessible active Cu sites, which energetically facilitate acetylene absorption and vinyl intermediate formation, thereby enabling efficient ethylene production at ampere-level current densities.
View Article and Find Full Text PDFNanomaterials (Basel)
December 2024
Copper-based materials, renowned for their redox versatility and conductivity, have extensive applications in electrochemical sensing. Herein, we construct stable Cu/Cu interfaces within dual-valence copper nanostructures to achieve enhanced sensitivity in glucose sensing. By employing a hydrolysis method to tune Cu/Cu ratios precisely, we achieved an optimal electrochemical interface with heightened stability and reactivity.
View Article and Find Full Text PDFSurface functionalization of Cu-based catalysts has demonstrated promising potential for enhancing the electrochemical CO reduction reaction (CORR) toward multi-carbon (C) products, primarily by suppressing the parasitic hydrogen evolution reaction and facilitating a localized CO/CO concentration at the electrode. Building upon this approach, we developed surface-functionalized catalysts with exceptional activity and selectivity for electrocatalytic CORR to C in a neutral electrolyte. Employing CuO nanoparticles coated with hexaethynylbenzene organic molecules (HEB-CuO NPs), a remarkable C Faradaic efficiency of nearly 90% was achieved at an unprecedented current density of 300 mA cm, and a high FE (> 80%) was maintained at a wide range of current densities (100-600 mA cm) in neutral environments using a flow cell.
View Article and Find Full Text PDFSci Bull (Beijing)
September 2024
Elastic strain in Cu catalysts enhances their selectivity for the electrochemical CO reduction reaction (eCORR), particularly toward the formation of multicarbon (C) products. However, the reasons for this selectivity and the effect of catalyst precursors have not yet been clarified. Hence, we employed a redox strategy to induce strain on the surface of Cu nanocrystals.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
August 2024
The practical application of the electrocatalytic CO reduction reaction (CORR) to form formic acid fuel is hindered by the limited activation of CO molecules and the lack of universal feasibility across different pH levels. Herein, we report a doping-engineered bismuth sulfide pre-catalyst (BiS-1) that S is partially retained after electrochemical reconstruction into metallic Bi for CORR to formate/formic acid with ultrahigh performance across a wide pH range. The best BiS-1 maintains a Faraday efficiency (FE) of ~95 % at 2000 mA cm in a flow cell under neutral and alkaline solutions.
View Article and Find Full Text PDFPeroxymonosulfate (PMS)-based advanced oxidation processes in liquid phase systems can actively degrade toluene. In this work, the catechol structural surfactant was introduced to synthesize the dispersed and homogeneous CoFeO nanospheres and embedded into MoS nanoflowers to form magnetically separable heterojunction catalysts. The innovative approach effectively mitigated the traditionally low reduction efficiency of transition metal ions during the heterogeneous activation process.
View Article and Find Full Text PDFThe field of small molecule electro-activated conversion is becoming a new star in modern catalytic research toward the carbon-neutral future. The advent of single-atom catalysts (SACs) is expected to greatly accelerate the kinetics of electrocatalytic reactions such as the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), hydrogen oxidation reaction (HOR), , owing to their maximum atomic efficiency, unique quantized energy level structure and strong interaction between well-defined active sites and supports. In this feature article, our group's proposed synthesis methodology applied in electrocatalysis is mainly summarized.
View Article and Find Full Text PDFAlthough noble metal nanocrystals have been studied extensively in the past decades, the shape-controlled synthesis of non-noble metal nanocrystals has remained challenging with limited success, which is a grand obstacle to their wide applications. Herein, a novel lattice mismatch-involved shape-control mechanism of Cu nanocrystals in a seed-mediated synthesis is reported, which can produce Cu nanoplates in high yield with tailored sizes (28-130 nm), holding great potential in optical and catalytic applications. The lattice mismatch between Cu and the seed is found effective in inducing crystallographic defects for symmetry breaking toward anisotropic nanocrystals.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2022
Atomically dispersed sites anchored on small oxide clusters are attractive new catalytic materials. Herein, we demonstrate an electrical pulse approach to synthesize atomically dispersed Pt on various oxide clusters in one step with nitrogen-doped carbon as the support (Pt -MO /CN). As a proof-of-concept application, Pt -FeO /CN is shown to exhibit high activity for oxygen reduction reaction (ORR) with a half-wave potential of 0.
View Article and Find Full Text PDFHematite (α-FeO) nanorod arrays grown on fluorine-doped tin oxide (FTO) substrate exhibit outstanding solar water splitting efficiency, benefiting from Sn self-doping induced by high-temperature annealing. However, this Sn self-doping couldn't be freely controlled without changing the optimized annealing conditions, which limits the further improvement of their photoelectrochemical (PEC) properties. Here, we report a facile hydrothermal synthesis with subsequent annealing approach to regulate the Sn diffusion via hafnium (Hf) doping as well as enhance the PEC performance of hematite photoanode.
View Article and Find Full Text PDFACS Appl Mater Interfaces
March 2022
Research (Wash D C)
January 2020
It is highly desirable, while still challenging, to obtain noble metal nanocrystals with custom capping ligands, because their colloidal synthesis relies on specific capping ligands for the shape control while conventional ligand exchange processes suffer from "the strong replaces the weak" limitation, which greatly hinders their applications. Herein, we report a general and effective ligand exchange approach that can replace the native capping ligands of noble metal nanocrystals with virtually any type of ligands, producing flexibly tailored surface properties. The key is to use diethylamine with conveniently switchable binding affinity to the metal surface as an intermediate ligand.
View Article and Find Full Text PDFACS Appl Mater Interfaces
October 2018
Ultra-small platinum nanoparticles loaded over titania is a promising catalyst for the low-temperature water-gas shift (WGS) reaction and shows the potential to work in a mobile hydrogen fuel cell system. Their precise size engineering (<3 nm) and reliable stabilization remain challenging. To address these issues, we report a reverse-micelle synthesis approach, which affords uniform ultra-small platinum nanoparticles (tunable in ∼1.
View Article and Find Full Text PDFChemistry
December 2018
Although hollow silver nanocrystals possess unique plasmonic properties, there is a lack of robust strategies to synthesize such nanocrystals with high efficiency and controllability. To solve this problem, a new surface-protected etching strategy to convert solid Ag nanocrystals, which are widely available from conventional syntheses, into their hollow counterparts, producing a family of hollow Ag nanocrystals is reported. Hollow Ag nanospheres and nanotubes were prepared conveniently in this way.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2018
Although aqueous synthesis of nanocrystals is advantageous in terms of the cost, convenience, environmental friendliness, and surface cleanness of the product, nanocrystals of Pt and non-noble metal alloys are difficult to obtain with controlled morphology and composition from this synthesis owing to a huge gap between the reduction potentials of respective metal salts. This huge gap could now be remedied by introducing a sulfite into the aqueous synthesis, which is believed to resemble an electroless plating mechanism, giving rise to a colloid of Pt-M (M=Ni, Co, Fe) alloy nanowires with an ultrasmall thickness (ca. 2.
View Article and Find Full Text PDFSelf-assembly at the nanoscale represents a powerful tool for creating materials with new structures and intriguing collective properties. Here, we report a novel strategy to synthesize nanoscale colloidosomes of noble metals by assembling primary metal nanoparticles at the interface of emulsion droplets formed by their capping agent. This strategy produces noble metal colloidosomes of unprecedentedly small sizes (<100 nm) in high yield and uniformity, which is highly desirable for practical applications.
View Article and Find Full Text PDFCreation of uniform sharp tips in noble metal nanostructures is highly desirable for chemical sensing applications that rely on their localized surface plasmon resonance (LSPR), while it remains a great challenge as typically it is not energetically favorable. Herein, we report a robust synthesis route to a novel family of unique shuriken-shaped Au nanostructures with four in-plane sharp tips in high yield and uniformity. The success of the synthesis relies on the anisotropic crystal growth of quasi-planar Au seeds by taking advantage of the capping effect of a ligand on the specific facets, as well as the predominant deposition of Au over its surface diffusion that accounts for the formation of the sharp tips.
View Article and Find Full Text PDFColloidal plasmonic metal nanoparticles have enabled surface-enhanced Raman scattering (SERS) for a variety of analytical applications. While great efforts have been made to create hotspots for amplifying Raman signals, it remains a great challenge to ensure their high density and accessibility for improved sensitivity of the analysis. Here we report a dealloying process for the fabrication of porous Au-Ag alloy nanoparticles containing abundant inherent hotspots, which were encased in ultrathin hollow silica shells so that the need of conventional organic capping ligands for stabilization is eliminated, producing colloidal plasmonic nanoparticles with clean surface and thus high accessibility of the hotspots.
View Article and Find Full Text PDF