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具有金属和非金属双掺杂调制的异常hcp Ni实现促进尿素氧化
Chemical Engineering Journal
(
IF
13.3
)
Pub Date : 2023-03-23
, DOI:
10.1016/j.cej.2023.142570
Ping Li
,
Yuqi Huang
,
Xiao Ouyang
,
Wenqin Li
,
Fengli Li
,
Shuanghong Tian
调制具有良好表面电子构型的具有成本竞争力的金属镍基电催化剂以促进尿素氧化反应 (UOR) 对尿素相关技术至关重要,但由于定制方法有限而极具挑战性。在此,我们提出了一种新的 N 掺杂诱导相转移策略,用金属 Co 和非金属 N 双掺杂工程 (hcp-CoNi-N/C) 构建反常亚稳态 hcp Ni,以控制电子态和对 UOR 的催化响应。令人印象深刻的是,hcp-CoNi-N/C 可以提供显着的 UOR 性能,与 RHE 相比具有 1.310 V 的极低电位,可达到 10 mA cm -2和快速反应动力学(34.0 mV dec –1), 在迄今为止报道的最好的 UOR 催化剂中脱颖而出。结合实验分析和理论计算表明,非常规的hcp相设计与金属和非金属双掺杂工程相结合,可以控制电子密度并产生有利于尿素吸附和C-N键断裂的电荷极化表面,从而显着促进尿素分解. 同时,这种协同相和掺杂工程可以通过调整润湿特性来提高传质动力学。这项研究提供了一种新的范例,通过与多种掺杂工程协同作用的不寻常的亚稳相设计来制备先进的金属镍基 UOR 催化剂。
"点击查看英文标题和摘要"
Unusual hcp Ni with metal and non-metal dual doping modulation to realize boosted urea oxidation
Modulating cost-competitive metallic Ni-based electrocatalysts with favorable surface electronic configuration to boost urea oxidation reaction (UOR) is crucial to urea-related technologies, yet dauntingly challenging due to limited tailoring methods. Herein we put forward a novel N-doping induced phase transfer strategy to construct anomalous metastable hcp Ni with metal Co and non-metal N dual doping engineering (hcp-CoNi-N/C) for manipulating electronic state and catalytic response toward the UOR. Impressively, the hcp-CoNi-N/C can deliver prominent UOR performance with an exceptionally low potential of 1.310 V vs. RHE to attain 10 mA cm−2 and fast reaction kinetics (34.0 mV dec–1), standing out among the best UOR catalysts reported to date. The combined experimental analysis and theoretical calculations disclose that unconventional hcp phase design coupled with metal and non-metal dual doping engineering enables electron density manipulation and creates a charge-polarized surface favorable for urea adsorption and C–N bond cleavage, thereby substantially promoting urea decomposition. Meanwhile, such synergistic phase and doping engineering can boost mass transfer kinetics via tailoring the wetting characteristics. This study offers a new paradigm to craft advanced metallic Ni-based UOR catalysts through unusual metastable phase design synergistic with multiple doping engineering.
更新日期:2023-03-23