“…Different from the bipolarized intrinsic faradaic layer on a semiconductor under illumination, the Pt and MnO x indicate only a mono-polarized faradaic layer, either the RFL or OFL, at a given potential. Therefore, intrinsic faradaic layers widely exist at the interfaces of semiconductor/liquid, metal/liquid and faradaic material/liquid, which form faradaic junctions [ 36 , 40 , 41 ]. According to the above discussion, the bipolarity or mono-polarity of the surface faradaic layer on a semiconductor depends on the applied potential in photoelectrocatalysis.…”
Interface charge transfer plays a key role in the performance of semiconductors for different kinds of solar energy utilization, such as photocatalysis, photoelectrocatalysis, photochromism and photo-induced superhydrophilicity. In previous studies, different mechanisms have been used to understand interface charge transfer process. However, the charge transfer mechanism at solid/liquid interface remains a controversial topic. Here, taking TiO2 as a model, we find and prove a new characteristic of photo-induced bipolarity of the surface layer (reduction faradaic layer and oxidation faradaic layer) on a semiconductor by experiments for the first time. Different from energy level positions in classic surface states transfer mechanism, the potential window of a surface faradaic layer locates out of the forbidden band. Moreover, we find that the reduction faradaic layer and oxidation faradaic layer serve as electron and hole transfer mediators in photocatalysis, while the bipolarity or mono-polarity of the surface layer on a semiconductor depends on the applied potential in photoelectrocatalysis. The new characteristic of bipolarity can also offer new insights on charge transfer process at semiconductor/liquid interface for solar energy utilization.
“…Different from the bipolarized intrinsic faradaic layer on a semiconductor under illumination, the Pt and MnO x indicate only a mono-polarized faradaic layer, either the RFL or OFL, at a given potential. Therefore, intrinsic faradaic layers widely exist at the interfaces of semiconductor/liquid, metal/liquid and faradaic material/liquid, which form faradaic junctions [ 36 , 40 , 41 ]. According to the above discussion, the bipolarity or mono-polarity of the surface faradaic layer on a semiconductor depends on the applied potential in photoelectrocatalysis.…”
Interface charge transfer plays a key role in the performance of semiconductors for different kinds of solar energy utilization, such as photocatalysis, photoelectrocatalysis, photochromism and photo-induced superhydrophilicity. In previous studies, different mechanisms have been used to understand interface charge transfer process. However, the charge transfer mechanism at solid/liquid interface remains a controversial topic. Here, taking TiO2 as a model, we find and prove a new characteristic of photo-induced bipolarity of the surface layer (reduction faradaic layer and oxidation faradaic layer) on a semiconductor by experiments for the first time. Different from energy level positions in classic surface states transfer mechanism, the potential window of a surface faradaic layer locates out of the forbidden band. Moreover, we find that the reduction faradaic layer and oxidation faradaic layer serve as electron and hole transfer mediators in photocatalysis, while the bipolarity or mono-polarity of the surface layer on a semiconductor depends on the applied potential in photoelectrocatalysis. The new characteristic of bipolarity can also offer new insights on charge transfer process at semiconductor/liquid interface for solar energy utilization.
“…The renewable-energy-powered electrochemical CO 2 reduction (CO 2 R) to value-added products is a promising solution for reducing the atmospheric CO 2 concentration and achieving sustainable carbon recycling. − Among the electrocatalysts for CO 2 R, copper (Cu)-based materials are unique candidates for the multi-electron reduction products (such as methane, ethylene, ethanol, etc. ) with appreciable activity. − However, the products of Cu-catalyzed CO 2 R are widely distributed, and the activity and selectivity for a specific product are still unsatisfactory. Therefore, it is of utmost significance to improve the catalytic activity, selectivity, and stability of Cu-based catalysts for their industrial applications. , …”
Copper (Cu), a promising catalyst for electrochemical CO 2 reduction (CO 2 R) to multi-electron reduction products, suffers from an unavoidable and uncontrollable reconstruction process during the reaction, which not only may lead to catalyst deactivation but also brings great challenges to the exploration of the structure−performance relationship. Herein, we present an efficient strategy for stabilizing Cu with silica and synthesize reconstruction-resistant CuSiO x amorphous nanotube catalysts with abundant atomic Cu−O−Si interfacial sites. The strong interfacial interaction between Cu and silica makes the Cu−O−Si interfacial sites ultrastable in the CO 2 R reaction without any apparent reconstruction, thus exhibiting high CO 2 -to-CH 4 selectivity (72.5%) and stability (FE CHd 4 remains above 60% after 12 h of test). A remarkable CO 2 -to-CH 4 conversion rate of 0.22 μmol cm −2 s −1 was also achieved in a flow cell device. This work provides a very promising route for the design of highly active and stable Cu-based CO 2 R catalysts.
“…[6][7][8][9] Among these methods, electrochemical CO 2 reduction (ECR) using water as a hydrogen source and renewable electricity as a driving force is an ideal solution to couple CO 2 utilization with renewable energy storage. [10][11][12][13][14] The ECR process will not bring additional CO 2 emissions, and the products obtained can usually be divided into two types: C 1 (such as CO, formic acid, methane, and methanol) and C 2+ (such as ethylene, ethanol, and n-propanol). These high-value-added products, in turn, can alleviate our dependence on traditional fossil fuels.…”
The renewable-energy-powered electrochemical CO2 reduction (ECR) is a promising way capable of transforming CO2 to value-added products and achieving sustainable carbon recycling. By virtue of the extremely high exposure rate...
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