Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2022-08-04 , DOI: 10.1016/j.apcatb.2022.121808
Nanzhu Nie , Dan Zhang , Zuochao Wang , Wenhao Yu , Shijie Ge , Juan Xiong , Yanli Gu , Bo Yang , Jianping Lai , Lei Wang
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Powerful, efficient, and corrosion-resistant electrocatalysts are in need to achieve high-current-density neutral seawater hydrogen evolution. Here, a novel strategy through strong metal-support interaction (SMSI) and incorporation of Pt to construct PtNb-Nb2O5 clusters @C was developed with stable high-current-density neutral seawater hydrogen evolution property for the first time. SMSI prevents agglomeration and corrosion of nanomaterials. Pt sites were proposed to play an anabranch role by binding H* to stabilize the Nb valence state and prevent water dissociation incapacitation. The optimized PtNb-Nb2O5 @CC delivers low overpotentials of 440 mV (500 mA cm−2) and 570 mV (1000 mA cm−2) in neutral seawater and has 360 h excellent durability at 500 mA cm−2. In-situ Fourier transform infrared spectroscopy (FTIR), in-situ Raman spectroscopies and theoretical calculations supported the hydrogen evolution reaction (HER) mechanism. PtNb-Nb2O5 heterogeneous interface provided more active sites for water dissociation. OH* adsorbed on Nb sites in stable Nb2O5, and H* adsorbed on Nb sites and desorbed as H2 on Pt sites in stable PtNb. Overall, this work not only first achieves stable high-current-density neutral seawater hydrogen evolution property, but also opens a new opportunity to explore SMSI and incorporation of Pt to prevent agglomeration, corrosion, and water dissociation incapacitation for catalytic applications under high current densities.
中文翻译:

用于高电流密度中性海水析氢的稳定 PtNb-Nb2O5 异质结构簇@CC
需要强大、高效和耐腐蚀的电催化剂来实现高电流密度的中性海水析氢。在这里,首次开发了一种通过强金属-载体相互作用(SMSI)和掺入Pt来构建PtNb-Nb 2 O 5簇@C的新策略,该策略具有稳定的高电流密度中性海水析氢特性。SMSI 可防止纳米材料的团聚和腐蚀。提出 Pt 位点通过结合 H* 来稳定 Nb 价态并防止水离解失能,从而发挥分枝作用。优化的 PtNb-Nb 2 O 5 @CC 提供 440 mV (500 mA cm -2 ) 和 570 mV (1000 mA cm -2) 在中性海水中,在 500 mA cm -2下具有 360 小时出色的耐用性。原位傅里叶变换红外光谱 (FTIR)、原位拉曼光谱和理论计算支持了析氢反应 (HER) 机制。PtNb-Nb 2 O 5异质界面为水解离提供了更多的活性位点。OH* 吸附在稳定的 Nb 2 O 5中的 Nb 位点上,H* 吸附在 Nb 位点上并以 H 2的形式解吸在稳定的 PtNb 中的 Pt 位点上。总体而言,这项工作不仅首先实现了稳定的高电流密度中性海水析氢性能,而且为探索 SMSI 和掺入 Pt 以防止高电流密度下催化应用的团聚、腐蚀和水离解失能提供了新的机会。 .