Nano Research ( IF 9.9 ) Pub Date : 2024-03-04 , DOI: 10.1007/s12274-024-6521-9 Guangbiao Cao , Haoran Xing , Haoguan Gui , Chao Yao , Yinjuan Chen , Yongsheng Chen , Xiazhang Li
Simultaneous conversion of CO2 and biomass into value-added chemicals through solar-driven catalysis holds tremendous importance for fostering a sustainable circular economy. Herein, plasmonic Bi quantum dots were immobilized on phosphoric acid modified attapulgite (P-ATP) nanorod using an in-situ reduction–deposition method, and were employed for photocatalytic reduction of CO2 coupled with oxidation of biomass-derived benzyl alcohol. Results revealed that Bi atoms successfully integrated into the basal structure of P-ATP, forming chemically coordinated Bi–O–Si bonds that served as efficient transportation channels for electrons. The incorporation of high-density monodispersed Bi quantum dots induced a surface plasmon resonance (SPR) effect, expanding the light absorption range into the near-infrared region. As a consequence, the photo-thermal transformation was significantly accelerated, leading to enhanced reaction kinetics. Notably, 50% Bi/P-ATP nanocomposite exhibited the highest plasmon-mediated photocatalytic CH4 generation (115.7 µmol·g−1·h−1) and CO generation (44.9 µmol·g−1·h−1), along with remarkable benzaldehyde generation rate of 79.5 µmol·g−1·h−1 in the photo-redox coupling system under solar light irradiation. The hydrogen protons released from the oxidation of benzyl alcohol facilitated the incorporation of more hydrogen protons into CO2 to form key CH3O− intermediates. This work demonstrates the synergistic solar-driven valorization of CO2 and biomass using natural mineral based catalyst.
中文翻译:
等离子体量子点调制纳米矿物以光热还原二氧化碳并结合生物质转化
通过太阳能驱动的催化作用将CO 2和生物质同时转化为增值化学品对于促进可持续循环经济具有极其重要的意义。在此,采用原位还原沉积方法将等离子体Bi量子点固定在磷酸改性凹凸棒石(P-ATP)纳米棒上,并用于光催化还原CO 2以及氧化生物质衍生的苯甲醇。结果表明,Bi 原子成功整合到 P-ATP 的基础结构中,形成化学配位的 Bi-O-Si 键,作为电子的有效传输通道。高密度单分散Bi量子点的结合引发了表面等离子体共振(SPR)效应,将光吸收范围扩大到近红外区域。结果,光热转化显着加速,导致反应动力学增强。值得注意的是,50% Bi/P-ATP 纳米复合材料表现出最高的等离激元介导的光催化 CH 4生成(115.7 µmol·g -1 ·h -1)和 CO 生成(44.9 µmol·g -1 ·h -1),以及在太阳光照射下,光氧化还原偶联体系中苯甲醛的生成率为79.5 µmol·g -1 ·h -1 。苯甲醇氧化释放的氢质子促进更多氢质子结合到CO 2中,形成关键的CH 3 O -中间体。这项工作展示了使用天然矿物基催化剂 对 CO 2和生物质进行太阳能驱动的协同增值。