Ma Hongyu, Wu Xi, Li Xinghua, Liu Jie, Dong Haipeng, Liu Yu, Niu Luyao, Zhang Fang, Wang Wenbo, Shao Changlu, Li Xiaowei, Liu Yichun
Center for Advanced Optoelectronic Functional Materials Research, and Key Laboratory of UV Light-Emitting Materials and Technology of Ministry of Education, Northeast Normal University, 5268 Renmin Street, Changchun 130024, People's Republic of China.
Inorg Chem. 2024 Aug 26;63(34):15735-15751. doi: 10.1021/acs.inorgchem.4c01643. Epub 2024 Aug 15.
Photocatalytic carbon dioxide (CO) reduction for high-value hydrocarbon fuel production is a promising strategy to tackle global energy demand and climate change. However, this technology faces formidable challenges, primarily stemming from low yield and poor selectivity of C2 products of the desired hydrocarbon fuels. This study reported ZnO/ZnCoO Janus hollow nanofibers (ZnO/ZCO JHNFs) prepared by electrospinning and atomic layer deposition. Photocatalytic tests revealed an ethanol yield of 4.99 μmol g h for ZnO/ZnCoO JHNFs, surpassing mixed ZnO/ZnCoO nanofibers (ZnO/ZCO NFs) by 4.35 times and pure ZnO by 12.7 times. The selectivity of 58.8% is 2.38 and 4.49 times higher than those of ZnO/ZnCoO NFs and ZnO, respectively. These enhancements are attributed to efficient carrier separation facilitated by the ordered internal electric field of the Z-scheme heterojunction interface, validated by the energy band evaluations from experimentation and density functional theory (DFT) simulations and charge separation characterizations of photocurrent, impedance, and photoluminescence spectra. The Janus structure also effectively exposes the surface of ZnCoO to CO molecules, increasing the active site availability, as confirmed by BET nitrogen adsorption/desorption, temperature-programmed desorption tests, and DFT adsorption energy calculations. This study proposes a novel approach for efficient photocatalytic hydrocarbon fuel production, with potential applications in energy and climate crisis mitigation.
光催化还原二氧化碳(CO)以生产高价值碳氢燃料是应对全球能源需求和气候变化的一项有前景的策略。然而,这项技术面临着巨大的挑战,主要源于所需碳氢燃料中C2产物的低产率和差的选择性。本研究报道了通过静电纺丝和原子层沉积制备的ZnO/ZnCoO双面中空纳米纤维(ZnO/ZCO JHNFs)。光催化测试表明,ZnO/ZnCoO JHNFs的乙醇产率为4.99 μmol g h,比混合的ZnO/ZnCoO纳米纤维(ZnO/ZCO NFs)高出4.35倍,比纯ZnO高出12.7倍。58.8%的选择性分别比ZnO/ZnCoO NFs和ZnO高2.38倍和4.49倍。这些增强归因于Z型异质结界面的有序内部电场促进的有效载流子分离,通过实验和密度泛函理论(DFT)模拟的能带评估以及光电流、阻抗和光致发光光谱的电荷分离表征得到验证。双面结构还有效地将ZnCoO的表面暴露于CO分子,增加了活性位点的可用性,这通过BET氮吸附/解吸、程序升温脱附测试和DFT吸附能计算得到证实。本研究提出了一种高效光催化碳氢燃料生产的新方法,在缓解能源和气候危机方面具有潜在应用。