Surface‐Regulated Rhodium–Antimony Nanorods for Nitrogen Fixation

Abstract

Surface regulation is an effective strategy to improve the performance of catalysts, but it has been rarely demonstrated for nitrogen reduction reaction (NRR) to date. Now, surface‐rough Rh2Sb nanorod (RNR) and surface‐smooth Rh2Sb NR (SNR) were selectively created, and their performance for NRR was investigated. The high‐index‐facet bounded Rh2Sb RNRs/C exhibit a high NH3 yield rate of 228.85±12.96 μg h−1 mg−1Rh at −0.45 V versus reversible hydrogen electrode (RHE), outperforming the Rh2Sb SNRs/C (63.07±4.45 μg h−1 mg−1Rh) and Rh nanoparticles/C (22.82±1.49 μg h−1 mg−1Rh), owing to the enhanced adsorption and activation of N2 on high‐index facets. Rh2Sb RNRs/C also show durable stability with negligible activity decay after 10 h of successive electrolysis. The present work demonstrates that surface regulation plays an important role in promoting NRR activity and provides a new strategy for creating efficient NRR electrocatalysts.

Folic Acid Self-Assembly Enabling Manganese Single-Atom Electrocatalyst for Selective Nitrogen Reduction to Ammonia

“…3d). Evidently, a double of notable peaks with a coupling constant of 72 Hz is detected using 15 and S16, six successive recycling tests at -0.45 V lead to no obvious fluctuation of NH 3 yield rate and FE for Mn-N-C SAC. Further, the catalyst exhibits no decrease in these values even after being subjected to a 10 h testing period (Figs.…”

“…Moreover, NRR involves multiple intermediates and needs to compete with the hydrogen evolution reaction (HER) in aqueous solution, which makes limited Faradaic efficiency (FE) for NH 3 [7][8][9][10][11][12][13][14]. Electrocatalysts based on precious metals like Ru and Rh have been experimentally and theoretically explored to present favorable NRR activity [6,[15][16][17][18]. From practical standpoint, it is significant to develop robust and selective electrocatalysts for NRR from cost-effective metals.…”

“…Before the electrochemical measurements, Nafion membrane was pretreated with 3 wt% hydrogen peroxide at 80 °C for 1 h, rinsed with deionized (DI) water and then soaked in DI at 80 °C for another 1 h. To remove the possible N contaminates, all the feeding gases including 14 N 2 (99.999%), 15 N 2 (99%) and Ar (99.999%) were subsequently passed through an alkaline trap of 0.1 M NaOH and an acidic trap of 0.05 M H 2 SO 4 . Before the experiment, the electrolyte was saturated with the purified Ar or N 2 for at least 30 min and the bubbled gas was maintained during the experiments.…”

“…Isotope labeling test was performed using the above-mentioned method with the feeding gas been changed to 15 N 2 enriched gas (99%). The formed 15 NH 3 in the electrolyte was examined by using 1 H NMR spectroscopy (nuclear magnetic resonance, 600 MHz).…”

Highly Active Hollow RhCu Nanoboxes toward Ethylene Glycol Electrooxidation

“…[5] Surprisingly, Pt/Pd/ Au-alternative EGOR electrocatalysts are rarely reported until now. According to previous reports, Rh nanomaterials are also excellent electrocatalyst and have been widely applied in many energy-related electrocatalytic reactions, including hydrazine oxidation reaction, [6] nitrogen reduction reaction, [7] oxygen evolution reaction, [8] and ammonia oxidation reaction, [1c] and so on. Especially, Rh-based nanomaterials show very high electroactivity for alcohol oxidation reactions, which even exceed Pt-based nanomaterials for some special electrocatalytic reaction, such as methanol oxidation reaction, [9] formic acid oxidation reaction, [10] ethanol oxidation reaction, [11] isopropanol oxidation reaction, [12] and so on.…”