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Rational Design of Silver Sulfide Nanowires for Efficient CO2 Electroreduction in Ionic Liquid
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-01-24 00:00:00 , DOI: 10.1021/acscatal.7b03619
Subiao Liu 1 , Hongbiao Tao 1 , Qi Liu 1 , Zhenghe Xu 1 , Qingxia Liu 1 , Jing-Li Luo 1
Affiliation  

Electroreduction of CO2 holds the promise for the utilization of CO2 and the storage of intermittent renewable energy. The development of efficient catalysts for effectively converting CO2 to fuels has never been more imperative. Herein, we successfully synthesized Ag2S nanowires (NWs) dominating at the facet of (121) using a modified facile one-step method and utilized them as a catalyst for electrochemical CO2 reduction reaction (CO2RR). Ag2S NWs in ionic liquid (IL) possess a partial current density of 12.37 mA cm–2, ∼14- and ∼17.5-fold higher than those of Ag2S NWs and bulk Ag in KHCO3, respectively. Moreover, it shows significantly higher selectivity with a value of 92.0% at the overpotential (η) of −0.754 V. More importantly, the CO formation begins at a low η of 54 mV. The good performance originates from not only the presence of [EMIM–CO2]+ complexes but also the specific facet contribution. The partial density of states (PDOS) and work functions reveal that the d band center of the surface Ag atom of Ag2S(121) is closer to the Fermi energy level and has a higher d-electron density than those of Ag(111) and Ag55, which lowers transition state energy for CO2RR. Besides, density functional theory (DFT) calculations indicate that the COOH* formation over Ag2S is energetically more favorable on (111) and (121) facets than that on Ag(111) and Ag55. Therefore, we conclude that the significantly enhanced performance of Ag2S NWs in IL synergistically originates from the solvent-assisted and specific facet-promoted contributions. This distinguishes Ag2S NWs in IL as an attractive and selective platform for CO2RR.

中文翻译:

离子液体中高效CO 2电还原的硫化银纳米线的合理设计

CO 2的电还原保留了利用CO 2和存储间歇性可再生能源的希望。迫切需要开发有效地将CO 2转化为燃料的高效催化剂。在这里,我们成功地使用改进的简便的一步法合成了在(121)晶面上占优势的Ag 2 S纳米线(NWs),并将其用作电化学CO 2还原反应(CO 2 RR)的催化剂。的Ag 2小号纳米线在离子液体(IL)具有的12.37毫安厘米的局部电流密度-2,~14-和~17.5倍比银更高2在KHCO小号纳米线和体积的Ag 3, 分别。此外,它显示出更高的选择性,在-0.754 V的过电势(η)处的选择性值为92.0%。更重要的是,CO的形成始于54 mV的低η。良好的性能不仅源于[EMIM–CO 2 ] +配合物的存在,还源于特定方面的贡献。状态的部分密度(PDOS)和功函数表明,Ag 2 S(121)表面Ag原子的d能带中心比费米能级更近,并且d电子密度比Ag(111)高。 )和Ag55,从而降低了CO 2 RR的过渡态能量。此外,密度泛函理论(DFT)计算表明,Ag 2上形成了COOH *S在(111)和(121)面上比在Ag(111)和Ag55上在能量上更有利。因此,我们得出结论,IL中Ag 2 S NWs的性能显着增强是由溶剂辅助的和特定的面促进的贡献协同产生的。这将IL中的Ag 2 S NWs区分为有吸引力的CO 2 RR选择性平台。
更新日期:2018-01-24
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