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Elaborately tailored NiCo2O4 for highly efficient overall water splitting and urea electrolysis
Green Chemistry ( IF 9.3 ) Pub Date : 2023-09-19 , DOI: 10.1039/d3gc01828h Yamei Wang 1, 2 , Lanli Chen 3 , Huaming Zhang 1 , Muhammad Humayun 2 , Junhong Duan 1 , Xuefei Xu 4 , Yanjun Fu 1 , Mohamed Bououdina 2 , Chundong Wang 2, 4
Green Chemistry ( IF 9.3 ) Pub Date : 2023-09-19 , DOI: 10.1039/d3gc01828h Yamei Wang 1, 2 , Lanli Chen 3 , Huaming Zhang 1 , Muhammad Humayun 2 , Junhong Duan 1 , Xuefei Xu 4 , Yanjun Fu 1 , Mohamed Bououdina 2 , Chundong Wang 2, 4
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For effective overall water splitting (OWS) in alkaline media, a novel Ru-doped bimetal oxide (Ru-NiCo2O4) catalyst deposited onto a conductive nickel foam (NF) is fabricated by a multi-step hydrothermal reaction, ion exchange, and subsequent annealing process. The distinctive 3D nanoneedle-like arrays not only provide an even distribution of Ru decorated NiCo2O4, but also expose additional active sites, facilitating electron transport and improving reaction kinetics. Besides, density functional theory (DFT) studies elucidate the electronic structure regulation in Ru-NiCo2O4 and the modification of the d-band center optimizes H* adsorption energy, which considerably increased the hydrogen production efficiency. Considering the aforementioned advantages, the as-prepared Ru-NiCo2O4 electrocatalyst exhibits greatly improved catalytic activity, requiring only 25 mV and 249 mV at 10 mA cm−2 for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), respectively, as well as robust stability. Amazingly, the Ru-NiCo2O4 electrode in a two-electrode alkaline electrolyzer only needs 1.55 V to produce 10 mA cm−2, making it more efficient than the commercial RuO2||Pt/C electrode (1.62 V). More importantly, 0.33 M urea only needs a low voltage of 1.427 V to drive the urine-mediated electrolysis, which is about 123 mV less than the urea-free electrolysis cell. This work presents an effective electronic structure engineering approach based on heteroatom doping that may be extended to design and fabricate novel high-performance OWS catalysts.
中文翻译：
精心定制的 NiCo2O4，用于高效整体水分解和尿素电解
为了在碱性介质中实现有效的整体水分解（OWS），通过多步水热反应、离子交换、沉积在导电泡沫镍（NF）上制备了一种新型掺钌双金属氧化物（Ru-NiCo 2 O 4 ）催化剂，以及后续的退火工艺。独特的3D纳米针状阵列不仅提供了Ru装饰的NiCo 2 O 4的均匀分布，而且还暴露了额外的活性位点，促进电子传输并改善反应动力学。此外，密度泛函理论（DFT）研究阐明了Ru-NiCo 2 O 4中的电子结构调控d带中心的修饰优化了H*吸附能，大大提高了产氢效率。考虑到上述优点，所制备的Ru-NiCo 2 O 4电催化剂表现出极大提高的催化活性，在10 mA cm -2下仅需要25 mV和249 mV即可进行析氢反应（HER）和析氧反应（OER） ，分别以及鲁棒稳定性。令人惊讶的是，双电极碱性电解槽中的Ru-NiCo 2 O 4电极仅需要 1.55 V 即可产生 10 mA cm -2，使其比商业 RuO 2更高效||Pt/C 电极 (1.62 V)。更重要的是，0.33 M尿素仅需要1.427 V的低电压来驱动尿液介导的电解，比无尿素电解池低约123 mV。这项工作提出了一种基于杂原子掺杂的有效电子结构工程方法，可以扩展到设计和制造新型高性能OWS催化剂。
更新日期：2023-09-20
中文翻译：
精心定制的 NiCo2O4，用于高效整体水分解和尿素电解
为了在碱性介质中实现有效的整体水分解（OWS），通过多步水热反应、离子交换、沉积在导电泡沫镍（NF）上制备了一种新型掺钌双金属氧化物（Ru-NiCo 2 O 4 ）催化剂，以及后续的退火工艺。独特的3D纳米针状阵列不仅提供了Ru装饰的NiCo 2 O 4的均匀分布，而且还暴露了额外的活性位点，促进电子传输并改善反应动力学。此外，密度泛函理论（DFT）研究阐明了Ru-NiCo 2 O 4中的电子结构调控d带中心的修饰优化了H*吸附能，大大提高了产氢效率。考虑到上述优点，所制备的Ru-NiCo 2 O 4电催化剂表现出极大提高的催化活性，在10 mA cm -2下仅需要25 mV和249 mV即可进行析氢反应（HER）和析氧反应（OER） ，分别以及鲁棒稳定性。令人惊讶的是，双电极碱性电解槽中的Ru-NiCo 2 O 4电极仅需要 1.55 V 即可产生 10 mA cm -2，使其比商业 RuO 2更高效||Pt/C 电极 (1.62 V)。更重要的是，0.33 M尿素仅需要1.427 V的低电压来驱动尿液介导的电解，比无尿素电解池低约123 mV。这项工作提出了一种基于杂原子掺杂的有效电子结构工程方法，可以扩展到设计和制造新型高性能OWS催化剂。
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