Science Bulletin
·
2020
·
IF 9.511
Dong-Rui Yang,Ling Liu,Qian Zhang,Yi Shi,Yue Zhou,Chungen Liu,Feng-Bin Wang,Xing-Hua Xia
Electrochemical conversion of CO 2 into fuels is a promising means to solve greenhouse effect and recycle chemical energy. However, the CO 2 reduction reaction (CO 2 RR) is limited by the high overpotential, slow kinetics and the accompanied side reaction of hydrogen evolution reaction. Au nanocatalysts exhibit high activity and selectivity toward the reduction of CO 2 into CO. Here, we explore the Faradaic efficiency (FE) of CO 2 RR catalyzed by 50 nm gold colloid and trisoctahedron. It is found that the maximum FE for CO formation on Au trisoctahedron reaches 88.80% at −0.6 V, which is 1.5 times as high as that on Au colloids (59.04% at −0.7 V). The particle-size effect of Au trisoctahedron has also been investigated, showing that the FE for CO decreases almost linearly to 62.13% when the particle diameter increases to 100 nm. The X-ray diffraction characterizations together with the computational hydrogen electrode (CHE) analyses reveal that the (2 2 1) facets on Au trisoctahedron are more feasible than the (1 1 1) facets on Au colloids in stabilizing the critical intermediate COOH*, which are responsible for the higher FE and lower overpotential observed on Au trisoctahedron.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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
·
环境科学
·
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
·
化学
·
环境科学
·
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
·
材料科学
·
环境科学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2023
·
IF 13.1
Jing Zhang,Jia-Jun Dai,De-Quan Cao,Heng Xu,Xing-Yu Ding,Chun-Hua Zhen,Beate Paulus,Jin-Yu Ye,Qian Liang,Jun-Ke Liu,Shi-Jun Xie,Sai-Sai Deng,Zhen Wang,Jun-Tao Li,Yao Zhou,Shi-Gang Sun
With tunable local electronic environment, high mass density of MN 4 sites, and ease of preparation, metal–organic conjugated coordinative polymer (CCP) with inherent electronic conductivity provides a promising alternative to the well-known M−N−C electrocatalysts. Herein, the coordination reaction between Cu 2+ and 1,2,4,5-tetraaminobenzene (TAB) was conducted on the surface of metallic Cu nanowires, forming a thin layer of CuN 4 -based CCP (Cu-TAB) on the Cu nanowire. More importantly, interfacial transfer of electrons from Cu core to the CuN 4 -based CCP nanoshell was observed within the resulting CuTAB@Cu, which was found to enrich the local electronic density of the CuN 4 sites. As such, the CuTAB@Cu demonstrates much improved affinity to the *COOH intermediate formed from the rate determining step; the energy barrier for C–C coupling, which is critical to convert CO 2 into C 2 products, is also decreased. Accordingly, it delivers a current density of −9.1 mA cm −2 at a potential as high as −0.558 V (vs. RHE) in H-type cell and a Faraday efficiency of 46.4% for ethanol. This work emphasizes the profound role of interfacial interaction in tuning the local electronic structure and activating the CuN 4 -based CCPs for efficient electroreduction of CO 2 .
研究领域:
材料科学
·
电化学
·
催化
·
能量转换
✓ 已验证
产品关联
DOI
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
·
催化
·
纳米技术
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-13
·
IF 16.6
Sun Ji Wei,Wu Xuefeng,Liu Peng Fei,Chen Jiacheng,Liu Yuanwei,Lou Zhen Xin,Zhao Jia Yue,Yuan Hai Yang,Chen Aiping,Wang Xue Lu,Zhu Minghui,Dai Sheng,Yang Hua Gui
Practical electrochemical CO 2 -to-CO conversion requires a non-precious catalyst to react at high selectivity and high rate. Atomically dispersed, coordinatively unsaturated metal-nitrogen sites have shown great performance in CO 2 electroreduction; however, their controllable and large-scale fabrication still remains a challenge. Herein, we report a general method to fabricate coordinatively unsaturated metal-nitrogen sites doped within carbon nanotubes, among which cobalt single-atom catalysts can mediate efficient CO 2 -to-CO formation in a membrane flow configuration, achieving a current density of 200 mA cm −2 with CO selectivity of 95.4% and high full-cell energy efficiency of 54.1%, outperforming most of CO 2 -to-CO conversion electrolyzers. By expanding the cell area to 100 cm 2 , this catalyst sustains a high-current electrolysis at 10 A with 86.8% CO selectivity and the single-pass conversion can reach 40.4% at a high CO 2 flow rate of 150 sccm. This fabrication method can be scaled up with negligible decay in CO 2 -to-CO activity. In situ spectroscopy and theoretical results reveal the crucial role of coordinatively unsaturated metal-nitrogen sites, which facilitate CO 2 adsorption and key *COOH intermediate formation.
研究领域:
材料科学
·
电化学
·
催化
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）