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Rational Regulation of Electronic Structure in Layered Double Hydroxide Via Vanadium Incorporation to Trigger Highly Selective CO2 Photoreduction to CH4
Small ( IF 13.0 ) Pub Date : 2022-08-07 , DOI: 10.1002/smll.202202334
Sha Yu 1 , Ling Tan 1 , Sha Bai 1 , Chenjun Ning 1 , Guihao Liu 1 , Huijuan Wang 1 , Bin Liu 1 , Yufei Zhao 1 , Yu-Fei Song 1
Affiliation  

To realize excellent selectivity of CH4 in CO2 photoreduction (CO2PR) is highly desirable, yet which is challenging due to the limited active sites for CH4 generation and severe electron-hole recombination on photocatalysts. Herein, based on the theoretically calculated effects of vanadium incorporation into the laminate of layered double hydroxides (LDHs), V into NiAl-LDH to synthesize a series of LDHs with various V contents is introduced. NiV-LDH is revealed to afford a high CH4 selectivity (78.9%), and extremely low H2 selectivity (only 0.4%) under λ > 400 nm irradiation. By further tuning the molar ratio of Ni to V, a CH4 selectivity of as high as 90.1% is achieved on Ni4V-LDH, and H2 is completely prohibited on Ni2V-LDH. Fine structural characterizations and comprehensive optical and electrochemical studies uncover V incorporation creates the lower-valence Ni species as active sites for generating CH4, and enhances the generation, separation, and transfer of photogenerated carriers.

中文翻译:

通过掺钒对层状双氢氧化物中电子结构的合理调控以触发高选择性 CO2 光还原为 CH4

在CO 2光还原(CO 2 PR)中实现CH 4的优异选择性是非常可取的,但由于光催化剂上产生CH 4的活性位点有限和严重的电子-空穴复合,这具有挑战性。在此,基于钒掺入层状双氢氧化物(LDHs)叠层的理论计算效果,将V引入NiAl-LDH以合成一系列不同V含量的LDHs。NiV-LDH在 λ > 400 nm 照射下可提供高 CH 4选择性(78.9%)和极低的 H 2选择性(仅 0.4%)。通过进一步调整 Ni 与 V 的摩尔比,CH 4对Ni 4 V-LDH的选择性高达90.1% ,在Ni 2 V-LDH上完全禁止H 2。精细的结构表征和全面的光学和电化学研究揭示了 V 的掺入创造了低价 Ni 物种作为产生 CH 4的活性位点,并增强了光生载流子的产生、分离和转移。
更新日期:2022-08-07
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