Transforming greenhouse gases such as CO₂ to energy rich carbon-based chemicals is considered as one of the most efficient technologies for environmental and energy sustainability. However, CO₂ is highly stable molecule and difficult to reduce due to its linear structure. The rate of reduction and the nature of fuel product depend on the kinetics and thermodynamics of involved reactions. While the overall reaction kinetics depends on the energy of activated CO₂ molecule and its subsequent transition states along with reduction dynamics. Here we demonstrate that by activation of thermodynamically stable CO₂ molecule through complexation or coordination with suitable activator such as N-heterocyclic polymers (e.g., poly(4-vinyl)pyridine, PVP), both the kinetics and thermodynamics of photoelectrochemical CO₂ reduction reaction can be controlled by proper choice of electrode materials and bias potential. We present a solar light driven photoelectrochemical process for producing formaldehyde and acetaldehyde selectively on multi-layered Cu/rGO/PVP/Nafion hybrid cathode.

将 CO ₂等温室气体转化为富含能量的碳基化学品被认为是实现环境和能源可持续性的最有效技术之一。然而，CO ₂是高度稳定的分子并且由于其线性结构而难以还原。还原速率和燃料产品的性质取决于相关反应的动力学和热力学。而整体反应动力学取决于活化的 CO ₂分子的能量及其随后的过渡态以及还原动力学。在这里，我们证明了通过激活热力学稳定的 CO ₂molecule through complexation or coordination with suitable activator such as N-heterocyclic polymers (eg, poly(4-vinyl)pyridine, PVP), both the kinetics and thermodynamics of photoelectrochemical CO ₂ reduction reaction can be controlled by proper choice of electrode materials and bias潜在的。我们提出了一种太阳能光驱动的光电化学工艺，可在多层 Cu/rGO/PVP/Nafion 混合阴极上选择性地生产甲醛和乙醛。