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Directional manipulation of electron transfer in copper/nitrogen doped carbon by Schottky barrier for efficient anodic hydrazine oxidation and cathodic oxygen reduction
Journal of Colloid and Interface Science ( IF 9.4 ) Pub Date : 2023-08-11 , DOI: 10.1016/j.jcis.2023.08.068
Qing Dong 1 , Yue Li 2 , Shan Ji 3 , Hui Wang 4 , Ze Kan 2 , Vladmir Linkov 5 , Rongfang Wang 6
Affiliation  

Development of bifunctional hydrazine oxidation and oxygen reduction electrocatalysts with high activity and stability is of great significance for the implementation of direct hydrazine fuel cells. Combining zero-dimensional metal nanoparticles with three-dimensional nitrogen-doped carbon nanosheets is an attractive strategy for balancing performance and cost. However, the precise construction of these composites remains a significant challenge, and thorough study of their interaction mechanisms is lacking. Herein, the CuNPs/CuSA-NPCF catalyst was constructed by anchoring copper nanoparticles on a three-dimensional nitrogen-doped porous carbon nanosheet framework through coordination of polyvinyl pyrrolidone and copper ions. The Schottky barrier of metal–semiconductor matched the Fermi level of the rectifying contact, thus enabling directional electron transfer. The resulting electron-deficient Cu nanoparticles surface exhibited Lewis acidity, which was beneficial to adsorption of hydrazine molecule. While the electron-enriched Cu–N4/carbon surface improved the adsorption of oxygen molecule, and accelerated electron supply from Cu-N4 active sites to various oxygen intermediates. The CuNPs/CuSA-NPCF Mott-Schottky catalyst exhibited excellent catalytic activity for hydrazine oxidation reaction and oxygen reduction reaction in an alkaline media. The directional manipulation of electron transfer in heterogeneous materials was an attractive universal synthesis method, providing new approach for the preparation of efficient and stable hydrazine fuel cell catalysts.



中文翻译:

通过肖特基势垒定向操纵铜/氮掺杂碳中的电子转移,以实现有效的阳极肼氧化和阴极氧还原

开发具有高活性和稳定性的双功能肼氧​​化和氧还原电催化剂对于直接肼燃料电池的实现具有重要意义。将零维金属纳米粒子与三维氮掺杂碳纳米片相结合是平衡性能和成本的一种有吸引力的策略。然而,这些复合材料的精确构建仍然是一个重大挑战,并且缺乏对其相互作用机制的深入研究。在此,通过聚乙烯吡咯烷酮和铜离子的配位,将铜纳米粒子锚定在三维氮掺杂多孔碳纳米片框架上,构建了Cu NPs /Cu SA -NPCF催化剂。金属-半导体的肖特基势垒与整流接触的费米能级匹配,从而实现定向电子转移。所得的缺电子Cu纳米粒子表面表现出Lewis酸性,有利于肼分子的吸附。而富电子的Cu-N 4 /碳表面改善了氧分子的吸附,并加速了Cu-N 4活性位点向各种氧中间体的电子供应。Cu NPs /Cu SA -NPCF Mott-Schottky 催化剂在碱性介质中对肼氧化反应和氧还原反应表现出优异的催化活性。异质材料中电子转移的定向调控是一种有吸引力的通用合成方法,为制备高效稳定的肼燃料电池催化剂提供了新途径。

更新日期:2023-08-15
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