Angew Chem Int Ed Engl
January 2025
Electrocatalytic urea synthesis from carbon dioxide (CO2) and nitrate (NO3-) offers a promising alternative to traditional industrial methods. However, current catalysts face limitations in the supplies of CO* and Nrelated* intermediates, and their coupling, resulting in unsatisfactory urea production efficiency and energy consumption. To overcome these challenges, we carried out tandem electrosynthesis approach using ruthenium dioxide-supported palladium-gold alloys (Pd2Au1/RuO2).
View Article and Find Full Text PDFBackground: Allergy to iodine contrast agents has long been a contraindication for balloon pulmonary angioplasty (BPA). We report the successful zero-contrast BPA procedure of a patient with inoperable chronic thromboembolic pulmonary hypertension (CTEPH) and severe iodine allergy using real-time fusion of computed tomography angiography (CTA) with x-ray fluoroscopy.
Case Presentation: A 62-year-old woman with CTEPH who developed a severe allergic reaction after the first BPA procedure.
It remains a grand challenge to develop electrocatalysts with simultaneously high activity, long durability, and low cost for the oxygen evolution reaction (OER), originating from two competing reaction pathways and often trade-off performances. The adsorbed evolution mechanism (AEM) suffers from sluggish kinetics due to a linear scaling relationship, while the lattice oxygen mechanism (LOM) causes unstable structures due to lattice oxygen escape. We propose a MoZnFeCoNi high-entropy alloy (HEA) incorporating AEM-promoter Mo and LOM-active Zn to achieve dual activation and stabilization for efficient and durable OER.
View Article and Find Full Text PDFElectrolyte alkaline cations can significantly modulate the reaction selectivity of electrochemical CO reduction (eCOR), enhancing the yield of the valuable multicarbon (C) chemical feedstocks. However, the mechanism underlying this cation effect on the C-C coupling remains unclear. Herein, by performing constant-potential AIMD simulations, we studied the dynamic behavior of interfacial K ions over Cu surfaces during C-C coupling and the origin of the cation effect.
View Article and Find Full Text PDFDesigning efficient catalysts for operating CO electroreduction in membrane electrode assembly (MEA) faces significant obstacles. Herein, we propose an asymmetrically coordinated Ni single-atom catalyst featuring axial Br coordination at NiNBr sites anchoring onto hollow Br/N co-doped carbon nanocages, achieved through a NaBr-assisted confined-pyrolysis strategy. The Ni-NBr-C catalyst exhibits a high CO Faradaic efficiency (FE>97 %) over the current density range of 50 to 350 mA cm in the MEA device.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2024
Aprotic Li-CO batteries suffer from sluggish solid-solid co-oxidation kinetics of C and LiCO, requiring extremely high charging potentials and leading to serious side reactions and poor energy efficiency. Herein, we introduce a novel approach to address these challenges by modulating the reaction pathway with tailored Pt d-electrons and develop an aprotic Li-CO battery with CO and LiCO as the main discharge products. Note that the gas-solid co-oxidation reaction between CO and LiCO is both kinetically and thermodynamically more favorable.
View Article and Find Full Text PDFMetal-support interaction (MSI) is pivotal and ubiquitously used in the development of next-generation catalysts, offering a pathway to enhance both catalytic activity and stability. However, owing to the lattice mismatch and poor solubility, traditional catalysts often exhibit a metal-on-support heterogeneous structure with limited interfaces and interaction and, consequently, a compromised enhancement of properties. Herein, we report a universal and tunable method for supersaturated doping of transition-metal carbides via strongly nonequilibrium carbothermal shock synthesis, characterized by rapid heating and swift quenching.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Single-atom catalysts with maximal atom-utilization have emerged as promising alternatives for chlorine evolution reaction (CER) toward valuable Cl production. However, understanding their intrinsic CER activity has so far been plagued due to the lack of well-defined atomic structure controlling. Herein, we prepare and identify a series of atomically dispersed noble metals (e.
View Article and Find Full Text PDFIron-nitrogen-carbon (Fe-N-C) catalysts, although the most active platinum-free option for the cathodic oxygen reduction reaction (ORR), suffer from poor durability due to the Fe leaching and consequent Fenton effect, limiting their practical application in low-temperature fuel cells. This work demonstrates an integrated catalyst of a platinum-iron (PtFe) alloy planted in an Fe-N-C matrix (PtFe/Fe-N-C) to address this challenge. This novel catalyst exhibits both high-efficiency activity and stability, as evidenced by its impressive half-wave potential () of 0.
View Article and Find Full Text PDFThere is notable progress in the development of efficient oxygen reduction electrocatalysts, which are crucial components of fuel cells. However, these superior activities are limited by imbalanced mass transport and cannot be fully reflected in actual fuel cell applications. Herein, the design concepts and development tracks of platinum (Pt)-nanocarbon hybrid catalysts, aiming to enhance the performance of both cathodic electrocatalysts and fuel cells, are presented.
View Article and Find Full Text PDFElectrosynthesis has emerged as an enticing solution for hydrogen peroxide (HO) production. However, efficient HO generation encounters challenges related to the robust gas-liquid-solid interface within electrochemical reactors. In this work, we introduce an effective hydrophobic coating modified by iron (Fe) sites to optimize the reaction microenvironment.
View Article and Find Full Text PDFDeveloping highly efficient and sustainable hydrogen evolution reaction (HER) electrocatalysts is important for the practical application of emerging energy technologies. The spherical structure and phosphorus-rich properties of Chlorella can facilitate the construction of comparable transition metal phosphide electrocatalysts. Here, a microorganism template strategy is proposed to construct a cobalt-phosphide-graphene hybrid.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
June 2024
The electrochemical CO reduction reaction (eCORR) to multicarbon products has been widely recognized for Cu-based catalysts. However, the structural changes in Cu-based catalysts during the eCORR pose challenges to achieving an in-depth understanding of the structure-activity relationship, thereby limiting catalyst development. Herein, we employ constant-potential density functional theory calculations to investigate the sintering process of Cu single atoms of Cu-N-C single-atom catalysts into clusters under eCORR conditions.
View Article and Find Full Text PDFDeveloping a high-performance membrane electrode assembly (MEA) poses a formidable challenge for fuel cells, which lies in achieving both high metal loading and efficient catalytic activity concurrently for MEA catalysts. Here, we introduce a porous Co@NC carrier to synthesize sub-4 nm PtCo intermetallic nanocrystals, achieving an impressive Pt loading of 27 wt %. The PtCo-CoNC catalyst demonstrates exceptional catalytic activity and remarkable stability for the oxygen reduction reaction.
View Article and Find Full Text PDFSeawater-flow- and -evaporation-induced electricity generation holds significant promise in advancing next-generation sustainable energy technologies. This method relies on the electrokinetic effect but faces substantial limitations when operating in a highly ion-concentrated environment, for example, natural seawater. We present herein a novel solution using calcium-based metal-organic frameworks (MOFs, CHCaO·2HO) for seawater-evaporation-induced electricity generation.
View Article and Find Full Text PDFSolar driven proton exchange membrane water electrolysis (PEMWE) is of great promise for stable and high-purity H production, but often limited by the serious partial loading issue due to the intermittent nature of solar energy, the kinetically sluggish oxygen evolution reaction (OER) and the usage of noble metal-based anodes (e. g., Pt, Ir, and Ru).
View Article and Find Full Text PDFThe high-current-density Zn-air battery shows big prospects in next-generation energy technologies, while sluggish O reaction and diffusion kinetics barricade the applications. Herein, the sequential assembly is innovatively demonstrated for hierarchically mesoporous molybdenum carbides/carbon microspheres with a tunable thickness of mesoporous carbon layers (Meso-MoC/C-x, where x represents the thickness). The optimum Meso-MoC/C-14 composites (≈2 µm in diameter) are composed of mesoporous nanosheets (≈38 nm in thickness), which possess bilateral mesoporous carbon layers (≈14 nm in thickness), inner MoC/C layers (≈8 nm in thickness) with orthorhombic MoC nanoparticles (≈2 nm in diameter), a high surface area of ≈426 m g, and open mesopores (≈6.
View Article and Find Full Text PDFDirect CO electroreduction to valuable chemicals is critical for carbon neutrality, while its main products are limited to simple C /C compounds, and traditionally, the anodic O byproduct is not utilized. We herein report a tandem electrothermo-catalytic system that fully utilizes both cathodic (i.e.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2023
The indirect electro-epoxidation of ethylene (C H ), produced from CO electroreduction (CO R), holds immense promise for CO upcycling to valuable ethylene oxide (EO). However, this process currently has a mediocre Faradaic efficiency (FE) due to sluggish formation and rapid dissociation of active species, as well as reductive deactivation of Cu-based electrocatalysts during the conversion of C H to EO and CO to C H , respectively. Herein, we report a bromine-induced dual-enhancement strategy designed to concurrently promote both C H -to-EO and CO -to-C H conversions, thereby improving EO generation, using single-atom Pt on N-doped CNTs (Pt /NCNT) and Br -bearing porous Cu O as anode and cathode electrocatalysts, respectively.
View Article and Find Full Text PDFElectrochemical carbon dioxide reduction reaction (CO RR) driven by renewable energy shows great promise in mitigating and potentially reversing the devastating effects of anthropogenic climate change and environmental degradation. The simultaneous synthesis of energy-dense chemicals can meet global energy demand while decoupling emissions from economic growth. However, the development of CO RR technology faces challenges in catalyst discovery and device optimization that hinder their industrial implementation.
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