Abstract:The ever-increasing concern for adverse
climate change
has stimulated
great research enthusiasm for CO2 conversion. The photocatalytic
CO2 reduction reaction (CO2RR) has become one
of the promising approaches to converting CO2 into value-added
fuels. However, CO2RR suffers from intense competition
from the hydrogen evolution reaction (HER) for electrons in aqueous
solution due to the limited mass transfer of CO2 in water.
In this study, we propose to construct the three-phase interface on
the photocatalyst sur… Show more
“…Designing an effective photocathode with an efficient interface to rapidly deliver electrons to the catalytic sites and large nanocages to enrich CO 2 presents a promising avenue for carbon dioxide fixation. 20,21 Herein, we propose a ZIF-8/ZnTe photocathode that is endowed with a zinc-sharing interface and CO 2 -collecting layer for efficient photoelectrochemical conversion of CO 2 into CO in nonaqueous solution. In this configuration, ZnTe acts as a light absorber and ZIF-8 serves as a membrane to selectively gather CO 2 molecules from the electrolyte and photogenerated electrons from ZnTe under illumination.…”
Section: Introductionmentioning
confidence: 99%
“…2000 m 2 ·g –1 ) and large number of active sites, , ZIF-8 has been employed as a cocatalyst for CO 2 reduction as well. Designing an effective photocathode with an efficient interface to rapidly deliver electrons to the catalytic sites and large nanocages to enrich CO 2 presents a promising avenue for carbon dioxide fixation. , …”
Artificial photosynthesis is an effective way of converting CO 2 into fuel and high value-added chemicals. However, the sluggish interfacial electron transfer and adsorption of CO 2 at the catalyst surface strongly hamper the activity and selectivity of CO 2 reduction. Here, we report a photocathode attaching zeolitic imidazolate framework-8 (ZIF-8) onto a ZnTe surface to mimic an aquatic leaf featuring stoma and chlorophyll for efficient photoelectrochemical conversion of CO 2 into CO. ZIF-8 possessing high CO 2 adsorption capacity and diffusivity has been selected to enrich CO 2 into nanocages and provide a large number of catalytic active sites. ZnTe with high light-absorption capacity serves as a light-absorbing layer. CO 2 molecules are collected in large nanocages of ZIF-8 and delivered to the ZnTe surface. As evidenced by scanning electrochemical microscopy, the interface can effectively boost interfacial electron transfer kinetics. The ZIF-8/ZnTe photocathode with unsaturated Zn−N x sites exhibits a high Faradaic efficiency for CO production of 92.9% and a large photocurrent of 6.67 mA•cm −2 at −2.48 V (vs Fc/Fc + ) in a nonaqueous electrolyte at AM 1.5G solar irradiation (100 mW•cm −2 ).
“…Designing an effective photocathode with an efficient interface to rapidly deliver electrons to the catalytic sites and large nanocages to enrich CO 2 presents a promising avenue for carbon dioxide fixation. 20,21 Herein, we propose a ZIF-8/ZnTe photocathode that is endowed with a zinc-sharing interface and CO 2 -collecting layer for efficient photoelectrochemical conversion of CO 2 into CO in nonaqueous solution. In this configuration, ZnTe acts as a light absorber and ZIF-8 serves as a membrane to selectively gather CO 2 molecules from the electrolyte and photogenerated electrons from ZnTe under illumination.…”
Section: Introductionmentioning
confidence: 99%
“…2000 m 2 ·g –1 ) and large number of active sites, , ZIF-8 has been employed as a cocatalyst for CO 2 reduction as well. Designing an effective photocathode with an efficient interface to rapidly deliver electrons to the catalytic sites and large nanocages to enrich CO 2 presents a promising avenue for carbon dioxide fixation. , …”
Artificial photosynthesis is an effective way of converting CO 2 into fuel and high value-added chemicals. However, the sluggish interfacial electron transfer and adsorption of CO 2 at the catalyst surface strongly hamper the activity and selectivity of CO 2 reduction. Here, we report a photocathode attaching zeolitic imidazolate framework-8 (ZIF-8) onto a ZnTe surface to mimic an aquatic leaf featuring stoma and chlorophyll for efficient photoelectrochemical conversion of CO 2 into CO. ZIF-8 possessing high CO 2 adsorption capacity and diffusivity has been selected to enrich CO 2 into nanocages and provide a large number of catalytic active sites. ZnTe with high light-absorption capacity serves as a light-absorbing layer. CO 2 molecules are collected in large nanocages of ZIF-8 and delivered to the ZnTe surface. As evidenced by scanning electrochemical microscopy, the interface can effectively boost interfacial electron transfer kinetics. The ZIF-8/ZnTe photocathode with unsaturated Zn−N x sites exhibits a high Faradaic efficiency for CO production of 92.9% and a large photocurrent of 6.67 mA•cm −2 at −2.48 V (vs Fc/Fc + ) in a nonaqueous electrolyte at AM 1.5G solar irradiation (100 mW•cm −2 ).
“…Therefore, the solid−liquid−gas three-phase interface at the cathode of the ZABs can also act as the gas-sensitive region, realizing the successful combination of the gas sensor and the energy supply device and overcoming the restriction of the external working environment, significantly promoting the miniaturization and integration of the sensing system. As compared to other electrochemical gas sensors such as mixed potential solid-electrolyte chemical gas sensors usually working at high working temperatures, the ZAB-based gas sensors can work at room temperature, which brings a smaller power consumption. , Moreover, the sensing response of the ZAB-based gas sensors is mainly determined by the electrochemical reaction at the solid−liquid−gas three-phase interface and the electric potential of the gas electrodes, , which will provide a better selectivity toward that of the traditional chemiresistive gas sensors. However, for the ZAB-based sensors, how to induce a huge and detectable voltage change to NO 2 gas with trace concentrations is still a challenge. 1 Working principle and application of the self-powered NO 2 sensor based on ZABs.…”
Exploration of novel self-powered gas sensors free of external energy supply restrictions, such as light illumination and mechanical vibration, for flexible and wearable applications is in urgent need. Herein, this work constructs a flexible and self-powered NO 2 gas sensor based on zinc-air batteries (ZABs) with the cathode of the ZABs also acting as the gas-sensitive layer. Furthermore, the SiO 2 coating film, serving as a hydrophobic layer, increases the three-phase interfaces for the NO 2 reduction reaction. The constructed sensors exhibit a high sensing response (0.3 V @ 5 ppm), an ultralow detection limit (61 ppb), a fast sensing process (129 and 103 s), and excellent selectivity. Moreover, the sensors also possess a wide working temperature range and a low working temperature tolerance (0.34 V at −15 °C). Simulations indicate that the hydrophobic surface at the cathode−hydrogel interface will accommodate more NO 2 gas molecules at the reaction sites and prevent the influence of inner water evaporation and direct dissolution of NO 2 in the electrolyte, which is beneficial to the enhanced gas sensing abilities. Finally, the self-powered sensing device is incorporated into a smart sensing system for practical applications. This work will pave a new insight into the construction of integrated and energy self-sufficient smart gas sensing systems.
Electrocatalytic carbon dioxide reduction reaction (CO2RR) has been recognized as a promising route to convert carbon emissions to high‐value chemicals and fuels. Significant breakthroughs are usually inseparable from deeper understanding of reaction mechanisms. To this end, molecular dynamics (MD) simulations have been invaluable in providing detailed insights into elucidation of complex reaction pathways and prediction of overall electrochemical performance, thus bridging macroscopic experimental observations and microscopic explanatory mechanisms. Directed by MD simulations, tremendous efforts have been devoted toward enhancing the CO2RR with rational design of electrocatalyst and efficient construction of electrode/electrolyte interface. Herein, a comprehensive review of applications of MD simulations in CO2RR is emerged. To begin with, specific fundamentals along with familiar methods such as algorithm and force fields of various MD simulations have been summed up. Followed, employment of MD simulations in optimization of CO2RR is introduced, encompassing interpretation of electrocatalyst activity, explanation of electrolyte effect, and investigation of electrode microenvironment. Definitively, imminent challenges and avenues for optimization in future MD simulations are contemplated, envisioning this review as a guiding beacon for future endeavors aimed at harnessing MD simulations to propel CO2RR toward a realm of heightened efficiency, economic viability, and practical utility.
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