多酸科學(xué)教育部重點(diǎn)實(shí)驗(yàn)室在利用多酸開(kāi)展電解水產(chǎn)氫研究領(lǐng)域取得重要進(jìn)展
氫能是清潔和理想的零碳排放能源之一。利用電催化分解水生產(chǎn)氫能具有能耗低、過(guò)程環(huán)保、產(chǎn)品純度高以及能量轉(zhuǎn)化效率高等優(yōu)點(diǎn)，是一種大有前景的能源存儲(chǔ)和轉(zhuǎn)化方式。其中最關(guān)鍵的問(wèn)題是尋找可替代貴金屬鉑的低成本、高活性的電催化劑。目前報(bào)道的大部分單組分電催化劑，其活性受限于自身固有的氫吸附自由能；而開(kāi)發(fā)多組分多界面復(fù)合型電催化劑有望改善材料的氫吸附能，并實(shí)現(xiàn)催化劑產(chǎn)氫性能的突破。近日，東北師范大學(xué)化學(xué)學(xué)院多酸科學(xué)教育部重點(diǎn)實(shí)驗(yàn)室在該領(lǐng)域取得重要研究進(jìn)展。
實(shí)驗(yàn)室博士生馬媛媛作為研究工作第一作者，博士后郎中玲作為共同第一作者，以過(guò)渡金屬取代型多酸作為催化劑分子設(shè)計(jì)平臺(tái)，利用多酸中天然的準(zhǔn)界面結(jié)構(gòu)原位塌陷，成功制備出一種納米尺寸多界面的鎳碳化物復(fù)合電催化劑Ni/WC@NC（如圖1所示）。這種多界面的Ni/WC@NC催化劑具備低成本、催化活性優(yōu)良、穩(wěn)定性好等優(yōu)點(diǎn)，可應(yīng)用于全pH范圍產(chǎn)氫。研究工作首次通過(guò)原位同步輻射實(shí)驗(yàn)、理論計(jì)算和旋轉(zhuǎn)環(huán)盤電極實(shí)驗(yàn)共同揭示了鎳與碳化鎢多界面結(jié)構(gòu)之間的電子轉(zhuǎn)移與質(zhì)子傳遞過(guò)程是催化劑提高活性的關(guān)鍵，而界面的增加將是復(fù)合型電催化劑性能提高的重要設(shè)計(jì)路徑。該工作發(fā)表于國(guó)際著名化學(xué)類雜志《能源與環(huán)境科學(xué)》上 (High efficient hydrogen evolution triggered by a multi-interfacial Ni/WC hybrid electrocatalyst, Energy Environ. Sci., 2018, 11, 2114 – 2123；IF = 30.067)，該論文是在李陽(yáng)光教授和譚華橋副教授研究團(tuán)隊(duì)指導(dǎo)下與蘇州大學(xué)康振輝和鐘俊教授課題組共同合作完成的。
圖1 由{Ni54W72}多酸制備Ni/WC@NC電催化劑用于電解水產(chǎn)氫研究
A New Progress in Polyoxometalate-Mediated High Efficient Noble-Metal-Free Electrocatalysts for Hydrogen Evolution Reaction
Hydrogen energy as a kind of zero-carbon emission energy has been considered as one of the cleanest energies. Hydrogen evolution reaction (HER) based on water electrolysis is a promising pathway for sustainable hydrogen production, owing to their low energy consumption, environmental-friendly process, pure products and high energy conversion efficiency. The important task in water splitting for hydrogen is developing low cost, high active and stable electrocatalysts. Recently, a research team in Northeast Normal University, Department of Chemistry has made an important breakthrough in this field.
The Ph. D student Yuan-yuan Ma as the first author and the postdoc Zhong-ling Lang as the co-first author employed the transition metal-substituted POM (Ni54W72) as precursor, which possess the natural quasi interfaces between different metal-oxo fragments in Ni54W72, and successfully prepared a new type of multi-interfacial nickel/tungsten carbide (Ni/WC) hybrid nanoparticles (NPs) anchoring on N-doped carbon sheets (Ni/WC@NC) (Figure 1). Such low-cost Ni/WC@NC electrocatalyst exhibits high activity and remarkable stability, and could be applied in wide range of pH. DFT calculations and in-situ XAS measurements reveal that the remarkable HER activity is mainly attributed to abundant interfaces between Ni and WC domains, which induces a synergistic optimization of the electronic configuration of Ni and WC through electron transfer process from WC to Ni along with potential mass transport, thus promoting the HER kinetics and accelerating the reaction. This work provides a new option for the design and preparation of promising HER electrocatalysts, and has been published in the flagship journal of RSC, Energy ＆ Environmental Science (High efficient hydrogen evolution triggered by a multi-interfacial Ni/WC hybrid electrocatalyst, Energy Environ. Sci., 2018, 11, 2114 - 2123). The correspondence authors are Professor Yang-Guang Li and associate Professor Hua-Qiao Tan from Northeast Normal University and Professor Zhen-Hui Kang and Jun Zhong from Soochow University.
Figure 1 Schematic view of the Ni/WC@NC prepared from {Ni54W72} POM as new type of HER electrocatalyst
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