当前位置：
X-MOL 学术
›
Adv. Funct. Mater.
›
论文详情
Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
Understanding Boosted Selective CO2-to-CO Photoreduction with Pure Water Vapor over Hierarchical Biomass-Derived Carbon Matrix
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-04-18 , DOI: 10.1002/adfm.202301785
Zhifeng Jiang 1 , Zhiquan Zhang 1 , Jianli Liang 2 , Min Zhou 1 , Daobin Liu 3 , Danjun Mao 4 , Qun Zhang 5 , Wei Zhang 1 , Huaming Li 1 , Li Song 3 , Taicheng An 6 , Po Keung Wong 6, 7 , Chun‐Sing Lee 2
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-04-18 , DOI: 10.1002/adfm.202301785
Zhifeng Jiang 1 , Zhiquan Zhang 1 , Jianli Liang 2 , Min Zhou 1 , Daobin Liu 3 , Danjun Mao 4 , Qun Zhang 5 , Wei Zhang 1 , Huaming Li 1 , Li Song 3 , Taicheng An 6 , Po Keung Wong 6, 7 , Chun‐Sing Lee 2
Affiliation
|
Solar-driven CO2 reduction reaction (CO2RR) with water into carbon-neutral fuels is of great significance but remains challenging due to thermodynamic stability and kinetic inertness of CO2. Biomass-derived nitrogen-doped carbon (N-Cb) have been considered as promising earth-abundant photocatalysts for CO2RR, although their activities are not ideal and the reaction mechanism is still unclear. Herein, an efficient catalyst is developed for CO2-to-CO conversion realized on diverse N-Cb materials with hierarchical pore structures. It is demonstrated that the CO2-to-CO conversion preferentially takes place on positively charged carbon atoms next to pyridinic-N using two representatives treated pollens with the largest difference in pyridinic-N density and N content as model photocatalysts. Systematic experimental results indicate that surface local electric field originating from charge separation can be boosted by hierarchical pore structures, doped N, as well as pyridinic-N. Mechanistic studies reveal that positively charged carbon atoms next to pyridinic-N serve as active sites for CO2RR, reduce the energy barrier on the formation of CO*, and facilitate the CO2RR performance. All these benefits cooperatively contribute to treated chrysanthemum pollen catalyst exhibiting excellent CO formation rate of 203.2 µmol h−1 g−1 with 97.2% selectivity in pure water vapor. These results provide a new perspective into CO2RR on N-Cb, which shall guide the design of nature-based photocatalysts for high-performance solar-fuel generation.
中文翻译：
了解在分层生物质衍生碳基质上使用纯水蒸气增强选择性 CO2 光还原为 CO
太阳能驱动的CO 2与水的还原反应（CO 2 RR）转化为碳中性燃料具有重要意义，但由于CO 2的热力学稳定性和动力学惰性，仍然具有挑战性。生物质源氮掺杂碳(NC b )被认为是地球上储量丰富的CO 2 RR光催化剂，但其活性并不理想且反应机制仍不清楚。在此，开发了一种有效的催化剂，用于在具有分级孔结构的多种NC b材料上实现CO 2至CO的转化。结果表明，CO 2使用吡啶-N密度和氮含量差异最大的两种代表性处理花粉作为模型光催化剂，α-CO转化优先发生在吡啶-N旁边带正电的碳原子上。系统的实验结果表明，分级孔结构、掺杂氮以及吡啶氮可以增强源自电荷分离的表面局域电场。机理研究表明，吡啶-N旁边带正电的碳原子可作为CO 2 RR的活性位点，降低CO*形成的能垒，并促进CO 2 RR性能。所有这些优点共同促进了处理后的菊花花粉催化剂表现出优异的 CO 形成速率（203.2 µmol h -1） g -1在纯水蒸气中的选择性为 97.2%。这些结果为NC b上的CO 2 RR提供了新的视角，这将指导用于高性能太阳能燃料发电的天然光催化剂的设计。
更新日期：2023-04-18
中文翻译：
了解在分层生物质衍生碳基质上使用纯水蒸气增强选择性 CO2 光还原为 CO
太阳能驱动的CO 2与水的还原反应（CO 2 RR）转化为碳中性燃料具有重要意义，但由于CO 2的热力学稳定性和动力学惰性，仍然具有挑战性。生物质源氮掺杂碳(NC b )被认为是地球上储量丰富的CO 2 RR光催化剂，但其活性并不理想且反应机制仍不清楚。在此，开发了一种有效的催化剂，用于在具有分级孔结构的多种NC b材料上实现CO 2至CO的转化。结果表明，CO 2使用吡啶-N密度和氮含量差异最大的两种代表性处理花粉作为模型光催化剂，α-CO转化优先发生在吡啶-N旁边带正电的碳原子上。系统的实验结果表明，分级孔结构、掺杂氮以及吡啶氮可以增强源自电荷分离的表面局域电场。机理研究表明，吡啶-N旁边带正电的碳原子可作为CO 2 RR的活性位点，降低CO*形成的能垒，并促进CO 2 RR性能。所有这些优点共同促进了处理后的菊花花粉催化剂表现出优异的 CO 形成速率（203.2 µmol h -1） g -1在纯水蒸气中的选择性为 97.2%。这些结果为NC b上的CO 2 RR提供了新的视角，这将指导用于高性能太阳能燃料发电的天然光催化剂的设计。
京公网安备 11010802027423号