Coupling with the nitrate electroreduction reaction (NitRR), the electrosynthesis of cyclohexanone oxime (CHO, the vital feedstock in the nylon-6 industry) from cyclohexanone provides a promising alternative to the traditional energy consumption process. However, it still suffers from low efficiency because selective production of *NHOH intermediate from NitRR under large current densities is challenging. We here report a CuMoO/nitrogen-doped carbon (NC) electrocatalyst with high-density Cu-Mo dual sites for NitRR to selectively produce and stabilize *NHOH, with the subsequent cyclohexanone oximation achieving the highest CHO Faradaic efficiency of 94.
View Article and Find Full Text PDFThe highly localized Fe d orbital in ion phthalocyanine (FePc)-based molecular catalysts significantly hinders their electrocatalytic nitrogen reduction reaction (eNRR) performance. Herein, we theoretically designed a series of FePc-based molecules with adjacent metal phthalocyanine sites to form an asymmetric delocalized electronic structure on Fe centers, promoting the catalytic activity and lowering the overpotential of the eNRR, as well as suppressing the hydrogen evolution reaction (HER) side reaction.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2024
Developing non-platinum group metal catalysts for the sluggish hydrogen oxidation reaction (HOR) is critical for alkaline fuel cells. To date, Ni-based materials are the most promising candidates but still suffer from insufficient performance. Herein, we report an unconventional hcp/fcc Ni (u-hcp/fcc Ni) heteronanocrystal with multiple epitaxial hcp/fcc heterointerfaces and coherent twin boundaries, generating rugged surfaces with plenty of asymmetric convex sites.
View Article and Find Full Text PDFContamination of per- and polyfluoroalkyl substances (PFAS) poses a significant threat to soil ecosystem health, yet there remains a lack of understanding regarding the responses of soil microbial communities to prolonged PFAS exposure in field conditions. This study involved a three-year field investigation to track changes in microbial communities and functions in soil subjected to the contamination of a primary PFAS, perfluorooctanoic acid (PFOA). Results showed that PFOA exposure altered soil bacterial and fungal communities in terms of diversity, composition, and structure.
View Article and Find Full Text PDFJOURNAL/nrgr/04.03/01300535-202419110-00030/figure1/v/2024-03-08T184507Z/r/image-tiff The inflammatory microenvironment and neurotoxicity can hinder neuronal regeneration and functional recovery after spinal cord injury. Ruxolitinib, a JAK-STAT inhibitor, exhibits effectiveness in autoimmune diseases, arthritis, and managing inflammatory cytokine storms.
View Article and Find Full Text PDFPhotodynamic therapy (PDT) has been approved for clinic. However, powerless efficiency for deep hypoxic tumor therapy remains an enormous challenge for PDT. Herein, a hypoxia-sensitive nanotherapeutic system (FTCD-SRGD) based on fullerene (C) and anoxic activating chemical prodrug tirapazamine (TPZ) is rationally designed for multimodal therapy of deep hypoxic tumors.
View Article and Find Full Text PDFThe thermally stable inorganic cesium-based perovskites promise efficient and stable photovoltaics. Unfortunately, the strong ionic bonds lead to uncontrollable rapid crystallization, making it difficult in fabricating large-area black-phase film for photovoltaics. Herein, we developed a facile hydrogen-bonding assisted strategy for modulating the crystallization of CsPbI Br to achieve uniform large-area phase-pure films with much-reduced defects.
View Article and Find Full Text PDFEco Environ Health
December 2022
After the Industrial Revolution, the ever-increasing atmospheric CO concentration has resulted in significant problems for human beings. Nearly all countries in the world are actively taking measures to fight for carbon neutrality. In recent years, negative carbon emission technologies have attracted much attention due to their ability to reduce or recycle excess CO in the atmosphere.
View Article and Find Full Text PDFElectrochemically converting CO back into fuels and chemicals is promising in alleviating the greenhouse effect worldwide. Various high-efficiency catalysts have been achieved, yet the unsatisfied structural stability under CO electrolysis conditions restricts their practical application. Herein, a sub-5 nm sized CuInS quantum dots (CIS-QDs) based electrocatalyst for converting CO into CO are developed.
View Article and Find Full Text PDFStructural engineering of nanomaterials offers a promising way for developing high-performance catalysts toward catalysis. However, the delicate modulation of thermodynamically unfavorable nanostructures with unconventional phases still remains a challenge. Here, the synthesis of hierarchical AuCu nanostructures is reported with hexagonal close-packed (2H-type)/face-centered cubic (fcc) heterophase, high-index facets, planar defects (e.
View Article and Find Full Text PDFThe alkaline hydrogen oxidation reaction (HOR) involves the coupling of adsorbed hydrogen (H) and hydroxyl (OH) species and is thus orders of magnitude slower than that in acid media. According to the Sabatier principle, developing electrocatalysts with appropriate binding energy for both intermediates is vital to accelerating the HOR though it is still challenging. Herein, we propose an unconventional bilateral compressive strained Ni-Ir interface (Ni-Ir()) as efficient synergistic HOR sites.
View Article and Find Full Text PDFElectrochemical CO reduction (ECR) to high-value multi-carbon (C) products is critical to sustainable energy conversion, yet the high energy barrier of C-C coupling causes catalysts to suffer high overpotential and low selectivity toward specific liquid C products. Here, the electronically asymmetric Cu-Cu/Cu-N-C (Cu/CuNC) interface site is found, by theoretical calculations, to enhance the adsorption of *CO intermediates and decrease the reaction barrier of C-C coupling in ECR, enabling efficient C-C coupling at low overpotential. The catalyst consisting of high-density Cu/CuNC interface sites (noted as ER-Cu/CuNC) is then accordingly designed and constructed on the high-loading Cu-N-C single atomic catalysts.
View Article and Find Full Text PDFAn electrochemical approach for ammonia production is successfully developed by coupling the anodic dinitrogen oxidation reaction (NOR) and cathodic hydrogen evolution reaction (HER) within a well-designed membraneless flow electrolyzer. The obtained reactor shows the preferential yield of ammonia over nitrogen oxides on the vanadium nitride catalyst surface. At an applied oxidation potential of 2.
View Article and Find Full Text PDFThe electrochemical carbon-dioxide reduction reaction (CORR) to high-value multi-carbon (C) chemicals provides a hopeful approach to store renewable energy and close the carbon cycle. Although copper-based catalysts with a porous architecture are considered potential electrocatalysts for CO reduction to C chemicals, challenges remain in achieving high selectivity and partial current density simultaneously for practical application. Here, the porous Cu catalysts with a cavity structure by in situ electrochemical-reducing CuO cavities are developed for high-performance conversion of CO to C fuels.
View Article and Find Full Text PDFJ Hazard Mater
February 2023
Understanding the fate and transport of perfluorooctanoic acid (PFOA) in soil and groundwater is essential to reliable assessments of its risks. This study investigated the impacts of Gram-positive Bacillus subtilis (BS), Gram-negative Pseudomonas aeruginosa (PA) and wild microbiota (WM) biofilm on the transport of PFOA in saturated sand columns at two ionic strengths (i.e.
View Article and Find Full Text PDFElectrocatalytic CO reduction driven by renewable energy has become a promising approach to rebalance the carbon cycle. Atomically dispersed transition metals anchored on N-doped carbon supports (M-N-C) have been considered as the most attractive catalysts to catalyze CO to CO. However, the sluggish kinetics of M-N-C limits the large-scale application of this type of catalyst.
View Article and Find Full Text PDFWe report herein the electrochemical scanning tunneling microscopy (ECSTM) study on the synergistic effect of Mg in CO reduction reaction (CORR) catalyzed by cobalt phthalocyanine (CoPc). ECSTM measurement molecularly resolves the self-assembled CoPc monolayer on the Au(111) substrate. In the CO environment, high-contrast species are observed in the adlayer and assigned to the CO adsorption on CoPc.
View Article and Find Full Text PDFElectrochemical reduction of CO into liquid fuels is a promising approach to achieving a carbon-neutral energy cycle but remains a great challenge due to the lack of efficient catalysts. Here, the hierarchical architectures assembled by ultrathin and porous S-modified Cu nanoflakes (Cu-S NFs) are designed and constructed as an efficient electrocatalyst for CO conversion to formate with high partial current density. Specifically, when integrated into a gas diffusion electrode in a flow cell, Cu-S NFs are capable of delivering the ultrahigh formate current density up to 404.
View Article and Find Full Text PDFControlling the architectures and crystal phases of metal@semiconductor heterostructures is very important for modulating their physicochemical properties and enhancing their application performances. Here, a facile one-pot wet-chemical method to synthesize three types of amorphous SnO -encapsulated crystalline Cu heterostructures, i.e.
View Article and Find Full Text PDFSingle-atom catalysts (SACs) are promising candidates to catalyze electrochemical CO reduction (ECR) due to maximized atomic utilization. However, products are usually limited to CO instead of hydrocarbons or oxygenates due to unfavorable high energy barrier for further electron transfer on synthesized single atom catalytic sites. Here we report a novel partial-carbonization strategy to modify the electronic structures of center atoms on SACs for lowering the overall endothermic energy of key intermediates.
View Article and Find Full Text PDFElectrochemical reduction of CO into value-added products is an effective approach to relieve environmental and energetic issues. Herein, EDTA anion-modified porous hollow copper microspheres (H-Cu MPs) were constructed by EDTA-2Na-assisted electrodeposition. The faradic efficiency (FE) of ethylene doubled from 23.
View Article and Find Full Text PDFElectrocatalytic CO reduction (ECR) is a promising technology to simultaneously alleviate CO -caused climate hazards and ever-increasing energy demands, as it can utilize CO in the atmosphere to provide the required feedstocks for industrial production and daily life. In recent years, substantial progress in ECR systems has been achieved by the exploitation of various novel electrode materials. The anodic materials and cathodic catalysts that have, respectively, led to high-efficiency energy input and effective heterogenous catalytic conversion in ECR systems are comprehensively reviewed.
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