Details

Autor(en) / Beteiligte

• Zhou, Yuzhuo
• Zhang, Wenlin
• Guo, Peng
• Guo, Yabo
• Zhan, Jiayu
• Wang, Yaheng
• Zhang, Bo
• Zhang, Shaobo
• Zhang, Lu-Hua
• Yu, Fengshou

Titel

Continuous regulation of Cu electronic states by rectifying Schottky contacts enhancing electrochemical nitrate reduction to ammonia

Ist Teil von

• Inorganic chemistry frontiers, 2024, Vol.11 (12), p.353-351

Ort / Verlag

London: Royal Society of Chemistry

Erscheinungsjahr

2024

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Electrochemical conversion of nitrate (NO 3 − ) to ammonia (NH 3 ) appears to be a carbon-neutral method to handle wastewater remediation, while providing an innovative pathway for high-value green ammonia synthesis. However, designing highly efficient electrochemical catalysts remains one of the primary challenges in fulfilling this strategy. Herein, we constructed a series of Cu@N x C metal-carbon Mott-Schottky heterostructures composed of Cu nanoparticles uniformly dispersed on tailorable N-doped carbon substrates. The broad range of the content of the N dopant greatly enables adjusting the band gap of the carbon. The increased N content leads to a higher degree of interfacial charge separation. The optimal heterostructured Cu@N 1.0 C electrocatalyst presents a FE NH 3 of 96.2% at −0.9 V vs. RHE and a remarkable NH 3 yield of 1353.1 mmol h −1 g cat −1 at −1.1 V vs. RHE, superior to those of the reference Cu@C and most of the reported NO 3 RR catalysts. The mechanism investigation demonstrates that rectifying Schottky contacts in the Cu@N x C heterostructures reduces the electron density of the Cu sites and further improves the Cu + concentration, thus promoting the adsorption and activation of NO 3 − . This study offers a new possibility for improving the NO 3 RR performance of electrocatalysts by the rectification strategy. Metal-carbon heterostructured Cu@N x C catalysts with precise regulation of the N content are constructed. The optimized Cu@N 1.0 C electrocatalyst converts NO 3 − to NH 3 with a high FE NH 3 of 96.2% at −0.9 V vs. RHE, and NH 3 yield rate is 1353.1 mmol h −1 g cat −1 at −1.1 V vs. RHE.