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1.
J Colloid Interface Sci ; 662: 786-795, 2024 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-38382363

RESUMO

Copper-based tandem catalysts are effective candidates for yielding multi-carbon (C2+) products in electrochemical reduction of carbon dioxide (CO2RR). However, these catalysts still face a significant challenge regarding in the low selectivity for the production of a specific product. In this study, we report a high selectivity of 77.8 %±2 % at -1.0 V (vs RHE) for the production of C2H4 by using a Cu88Ag12NW catalyst which is primarily prepared through a combined Cu-Ag co-deposition and wet chemical method, employing an attractive strategy focused on regulating the microenvironment over Cu-Ag nanowires. The experimental and computational studies show that the higher *CO coverage and lower intermediate adsorption energy are important reasons for achieving the high C2H4 selectivity of Cu88Ag12NW catalyst. Comsol simulation results indicate that dense nanowires exhibit a nano-limiting effect on OH- ions, thereby leading to an increase in local pH and promoting coupling reactions. The catalyst demonstrates no noticeable decrease in current density or selectivity even after 12 h of continuous operation. The Cu-Ag nanowire composite exhibits remarkable catalytic activity, superior faradaic efficiency, excellent stability, and easy synthesis, which highlights its significant potential for electro-reducing carbon dioxide into valuable products.

2.
J Colloid Interface Sci ; 631(Pt B): 173-181, 2023 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-36401925

RESUMO

Enhancing the electrocatalytic oxygen evolution reaction (OER) performance is essential to realize practical energy-saving water electrolysis and CO2 electroreduction. Herein, we report a bimetallic co-doping engineering to design and fabricate nickel-cobalt-iron collaborative oxy-hydroxide on nickel foam that labeled as NiCoFeOxHy-NF. As expected, NiCoFeOxHy-NF exhibits an outstanding OER activity with current density of 10 mA cm-2 at 194 mV, Tafel slope of 53 mV dec-1, along with the robust long-term stability, which is significantly better than bimetallic NiCo and NiFe combinations. Comprehensive computational simulations and characterizations jointly unveil that the twisted ligand environment induced by heteroatoms ensures the balance strength between the metal-oxygen hybrid orbital states and the oxidized intermediates adsorption, thus lowering the oxygen cycling energy barriers for overcoming the sluggish OER kinetics. Moreover, a novel phase transition behavior is monitored by in-situ Raman spectra under OER operating conditions, which facilitates electron-mass transfer as well as boosts the exposure of activity sites. For practical applications, Ni2P-NF || NiCoFeOxHy-NF and Cu || NiCoFeOxHy-NF couples were constructed to realize high-efficiency water electrolysis and CO2 electrochemical reduction for the production of valuable H2 and C2H4, respectively. This work elucidates a novel mechanism by which bimetallic co-doping improves the electrocatalytic OER activity of nickel-based hydroxides.

3.
Nanomaterials (Basel) ; 9(6)2019 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-31159486

RESUMO

A novel strategy for large-scale synthesis of ZnO nanowire film is reported, which inherits the advantages of the solution-phase method and seeded growth process, such as low-temperature, efficient, economical, facile and flexible. It is easy to implement on various metals through room-temperature electrodeposition, followed by hydrothermal treatment at 90 °C, and suitable for industrialized production. The ZnO nanowires with an average wire diameter about 40 nm are in situ grown from and on nanocrystalline zinc coating, which forms a strong metallurgical bonding with the substrates. The p-type ZnO nanowire film has a well-preferred orientation along the (100) direction and a wurtzite structure, thereby displaying an effective photocatalytic capability for carcinogenic Cr6+ ions and CO2 greenhouse gas reduction under visible light irradiation. In addition to these features, the ZnO nanowire film is easy to recycle and, therefore, it has broad application prospects in contaminant degradation and renewable energy.

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