FeOOH have received considerable attention due to their natural abundance and cost-effectiveness. Despite the significant progress achieved, the one-step synthesis of integrated FeOOH is still a major challenge. Meanwhile, the current research on FeOOH catalyst still suffers from the unclear mechanism of controlling morphology. Here, density functional theory (DFT) calculations and X-ray photoelectron spectroscopy (XPS) demonstrated the strong electron-capturing and hydrogen absorption ability of Co in FeOOH, which further promotes the formation and stabilization of FeOOH. We used a one-step electrodeposition method to synthesize Co introduced FeOOH integrated electrocatalyst and propose to introduce ions with different valence states to regulate the morphology of FeOOH by precise modulation of electric double layer (EDL) composition and thickness. The prepared Co-FeOOH-K+ has a larger electrochemically active surface area (ECSA) (325 cm2) and turnover frequency (TOF) value (0.75 s−1). In the electrochemical experiments of an alkaline anion exchange membrane electrolyzer, Co-FeOOH-K+ shows better oxygen evolution performance than commercial RuO2 under industrial production conditions and has good industrial application prospects.
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The main problem faced by ethanol oxidation reaction (EOR) includes low activity, poor selectivity, and durability. In the study, we found that polysulfide modified on the surface of PtCu intermetallic (IM)/C can simultaneously enrich hydroxyl and ethanol, which could effectively improve the catalytic activity, CO2 selectivity, and durability of catalyst. The mass activity and the specific activity of the product in 1 M KOH electrolyte reached 17.83 A·mgPt−1 and 24.67 mA·cm−2. The CO2 selectivity of polysulfide modified product achieved 93.5%, which was 30 folds higher than Pt/C. In addition, the catalyst showed high catalytic stability. The mechanism study demonstrates that the surface modified polysulfide could significantly boost the enrichment effect of ethanol and hydroxyl species, accelerating C–C bond cleavage and CO oxidation.
Coordination engineering can enhance the activity and stability of the catalyst in heterogeneous catalysis. However, the axial coordination engineering between different groups on the carbon carrier and molecular catalysts in the electrocatalytic carbon dioxide reduction reaction (CO2RR) has been studied rarely. Through coordination engineering strategy, a series of amino (NH2), hydroxyl (OH), and carboxyl (COOH) groups functionalized carbon nanotubes (CNT) immobilized cobalt phthalocyanine (CoPc) catalysts are designed. Compared with no groups, OH groups and COOH groups, NH2 groups can effectively change the coordination environment of the central metal Co, thereby significantly increasing the turnover frequency (TOF) (31.4 s−1 at −0.6 V vs. RHE, CoPc/NH2-CNT > CoPc/OH-CNT > CoPc/COOH-CN > CoPc/CNT). In the flow cell, the CoPc/NH 2-CNT catalyst has high carbon monoxide (CO) selectivity at high current density (~ 100% at −225 mA·cm−2, ~ 96% at −351 mA·cm−2). Importantly, the CoPc/NH2-CNT catalyst can operate stably for 100 h at 225 mA·cm−2. Theoretical calculations reveal that CoPc/NH2-CNT catalyst is beneficial to the formation of *COOH and desorption of *CO, thus promoting CO2RR. This work provides an excellent platform for understanding the effect of coordination engineering on electrocatalytic performance and promotes a way to explore efficient and stable catalysts in other applications.