JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Jia Li,Yang Li,Yingshan Zeng,Yang Liu,Zhengguo Song,Zhi Liu
CO 2 photo reduction provides a feasible technique to solve climate issues and promote carbon neutrality. However, the efficiency of CO 2 photo reduction is severely depressed by the rapid recombination of photo generated carriers within photo catalysts, restricting the participation of electrons in the reduction process. In this study, we successfully construct a two-dimensional (2D) multilayer internal electric field (IEF) heterostructure by engineering the interface between NiAl-LDH and ZnV 2 O 6 (ZNA). Driven by the IEF, the separation of photo generated electron-hole pairs is significantly enhanced, leading to the increased utilization efficiency of carriers for active sites. The best-performing sample of ZNA-2 achieves a highest CO yield of 695.8 μmol g −1 , approximately 30.5-fold higher than that of pristine ZnV 2 O 6 . Photo electrochemical measurement and density functional theory (DFT) calculation results reveal that the 2D-2D stacked structure generates multiple interlayer built-in electric fields, which are crucial for enhancing carrier separation and suppressing recombination. Adsorption energy and intermediate COOH* analysis reveal that ZNA-2 significantly lowers the adsorption energy of CO 2 , promoting its stable adsorption and subsequent conversion. Moreover, the unique 2D multilayer IEF heterostructure greatly facilitates the formation of key intermediate COOH* and the desorption of CO during CO 2 photo reduction, leading to high CO activity and selectivity. The present work discloses the unprecedented potential of 2D multilayer IEF heterostructures for efficient CO 2 photo reduction, marking a significant advancement over conventional 2D counterparts.
研究领域:
材料科学
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环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2021
·
IF 3.626
Jianan Li,Wenbo Sun,Xinyong Li,Hangfan Ma,Yaxuan Li,Chong Peng
Photocatalysis is an effective means to convert CO 2 and solar energy into high value-added chemicals. Herein, the surface gradient S doped CuCo 2 O 4 microflowers were fabricated by an in situ topotactic engineering strategy. This photocatalyst presented CO 2 photoreduction with a satisfying activity (5 h, 181 μmol) and stability (94.5% retention). Additionally, the theoretical calculations indicated the fomated M-S bond could be favorbale to facilitate the initial CO 2 ⁎ binding and promote the formation of COOH ⁎ intermediates. This work provides a novel strategy for the fabrication of effective photocatalysts and highlights an in-depth understanding of micro-level regulation towards photocatalytic overall performance.
研究领域:
材料科学
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化学
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环境科学
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纳米技术
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Zhai Jianxin,Xia Zhanghui,Zhou Baowen,Wu Haihong,Xue Teng,Chen Xiao,Jiao Jiapeng,Jia Shuaiqiang,He Mingyuan,Han Buxing
Upcycling of CO 2 into fuels by virtually unlimited solar energy provides an ultimate solution for addressing the substantial challenges of energy crisis and climate change. In this work, we report an efficient nanostructured Ru/MnO x catalyst composed of well-defined Ru/MnO/Mn 3 O 4 for photo-thermal catalytic CO 2 hydrogenation to CH 4 , which is the result of a combination of external heating and irradiation. Remarkably, under relatively mild conditions of 200 °C, a considerable CH 4 production rate of 166.7 mmol g −1 h −1 was achieved with a superior selectivity of 99.5% at CO 2 conversion of 66.8%. The correlative spectroscopic and theoretical investigations suggest that the yield of CH 4 is enhanced by coordinating photon energy with thermal energy to reduce the activation energy of reaction and promote formation of key intermediate COOH* species over the catalyst. This work opens up a new strategy for CO 2 hydrogenation toward CH 4 .
研究领域:
化学
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材料科学
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环境科学
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能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2025
·
IF 6.3
Cong Li,Nuramina Abdukirim,Tursun Abdiryim,Ruxangul Jamal,Feng Xu,Yaoming Yu,Sihuleng Ba
Oxygen vacancy (V O ) engineering is an effective strategy for enhancing the performance of electrocatalytic CO 2 reduction (eCO 2 RR) to CO. In this study, composite materials of zinc oxide (ZnO) and polypyrrole (PPy) were prepared via in situ polymerization, with the V O concentration precisely controlled by adjusting the PPy molar ratio. The V O concentration first increased and then decreased as the PPy content decreased, while the zinc vacancy (V Zn ) concentration exhibited an opposite trend. Characterization results indicate that the PPy conjugated framework dynamically regulates the V O /V Zn concentration through electron injection, and its controllable hydrophobicity enhances CO 2 mass transfer and interfacial enrichment. Crucially, experiments reveal that a high V O concentration is key to achieving high performance, as V O reduces the activation energy barrier for C O bond cleavage through charge redistribution, synergistically optimizing the adsorption energy of the *COOH intermediate. Density functional theory calculations confirm that Vo regulates the d-band center position of ZnO and reduces the activation energy barrier for CO 2 activation. The optimal sample, V O -enriched ZnO/PPy-4, achieves an FE CO of 73.8 % at −1.6 V (vs. RHE) and stably maintains CO/H 2 ratio of 2:1 at −1.2 V (vs. RHE), with < 5 % decay rover 8 h. This study demonstrates a strategy for obtaining high-performance electrocatalytic CO 2 reduction catalysts by regulating Vo concentration.
研究领域:
材料科学
·
电化学
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催化
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纳米技术
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环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
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