揭示晶面定制氧化钴-rGO异质结构对二氧化碳选择性还原为乙醇的电催化活性,ACS Applied Nano Materials

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揭示晶面定制氧化钴-rGO异质结构对二氧化碳选择性还原为乙醇的电催化活性
ACS Applied Nano Materials ( IF 5.3 ) Pub Date : 2022-08-09 , DOI: 10.1021/acsanm.2c01703
Suparna Saha ₁ , Soumyajit Maitra ₂ , Mausumi Chattopadhyaya ₃ , Arundhati Sarkar ₁ , Suhail Haque ₁ , Subhasis Roy ₂ , Kajari Kargupta ₁

Affiliation

研究了锚定在还原氧化石墨烯 (rGO) 片上的 Co ₃ O ₄纳米晶体 (NC)的形态调制和晶面定制的电催化活性，用于将二氧化碳 (CO ₂ ) 选择性还原为 C2 产物。通过调整钴与 GO 的比例，合成了在rGO 上以四面体 Co(II) 为主的 Co ₃ O _{4 (111) 晶面的特殊设计的互连纳米网络。}_{rGO-Co 3} O ₄的结构性质通过高分辨率透射电子显微镜、扫描电子显微镜、X 射线衍射、电化学阻抗谱 (EIS)、X 射线光电子能谱 (XPS) 和 Brunauer-Emmett-Teller (BET) 技术分析复合材料。乙醇和乙烯的法拉第效率 (FE) 分别达到最大值 45.9 和 28.8%，最佳电位为 -0.4 V vs RHE（FE_{乙醇/乙烯}= 1.7）。密度泛函理论 (DFT) 揭示了 Co ₃ O _{4和石墨烯在互连形态下的强 dΠ-pΠ 相互作用，与原始 Co}₃ O ₄相比，这增加了异质结构的杂化以及电子导电性（由 EIS 和 XPS 分析支持），导致石墨烯片变形。_{(111) 晶面 Co 3} O ₄ NCs 的四面体 Co(II) 和八面体 Co(III) 上的相邻中间体之间的电位差促进 C-C 耦合并通过类似电路的机制增强多电子传输乙醇的合成。我们探索了对 CO ₂还原的显着反应性不仅与 Co ₃ O ₄的 wt% 相关，而且还与它在 rGO 上的形态模式有关，它控制促进乙醇形成的反应中间体 (*CO) 吸附位点。

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Unveiling the Electrocatalytic Activity of Crystal Facet-Tailored Cobalt Oxide-rGO Heterostructure Toward Selective Reduction of CO2 to Ethanol

Morphology-modulated and crystal facet-tailored electrocatalytic activity of Co₃O₄ nanocrystals (NCs) anchored on the reduced graphene oxide (rGO) sheet is explored for selective reduction of carbon dioxide (CO₂) to C2 products. Specially engineered interconnected nanonetwork of the Co₃O₄ (111) facet dominated by tetrahedral Co(II) on rGO is synthesized by tuning the cobalt to GO ratio. The structural properties of of rGO–Co₃O₄ composite is analyzed by high-resolution transmission electron microscopy, scanning electron microscopy, X-ray diffraction, electrochemical impedance spectroscopy (EIS), X-ray photoelectron spectroscopy (XPS), and Brunauer–Emmett–Teller (BET) techniques. Faradaic efficiencies (FE) of ethanol and ethylene attain the maximum value of 45.9 and 28.8%, respectively, at the optimum potential of −0.4 V vs RHE (FE_{ethanol/ethylene} = 1.7). The density functional theory (DFT) reveals strong dΠ–pΠ interactions between Co₃O₄ and graphene at interconnected morphology, which increases hybridization as well as electronic conductivity of the heterostructure compared to pristine Co₃O₄ (as supported by EIS and XPS analyses), causing deformation on the graphene sheet. The potential difference between the adjacent intermediates attached on tetrahedral Co(II) and octahedral Co(III) of (111) faceted Co₃O₄ NCs promote the C–C coupling and enhance the multi-electron transport through a circuit-like mechanism for the synthesis of ethanol. We explored that notable reactivity toward CO₂ reduction is not solely associated with wt % of Co₃O₄ but also the morphological pattern of it on rGO that control the reaction intermediate (*CO) adsorption sites facilitating ethanol formation.

更新日期：2022-08-09

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