APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Jianhao Li,Zhicheng Hu,Shuhuan Han,Dapeng Cao,Xiaofei Zeng,Jianfeng Chen
Electrocatalytic CO 2 reduction reaction (CO 2 RR) to multi-carbon product, especially for ethylene (C 2 H 4 ), provides a favorable pathway for carbon neutrality and renewable energy storage. However, the second-order C-C coupling reactions in CO 2 RR need always the high activation/driven energy in dynamics originating from the trace C 1 intermediate product. Herein, we synthesized the Ag-decorated Cu 2 O porous hollow core-shell catalyst named Ag@Cu 2 O where Ag nanoparticles uniformly distributed on inner the surface of the hollow Cu 2 O (H-Cu 2 O) via the sacrificial template method. Benefiting from the synergistic hollow structure and electron transfer from Cu and Ag to O, Ag@Cu 2 O catalyst delivers the excellent C 2 H 4 Faradaic Efficiency (FE) of 55 % ± 2 % at −1.0 V (vs. RHE), which is superior to the most reported catalysts. More importantly, in situ infrared spectroscopy and density functional theory (DFT) calculations reveal the introduction of Ag can decrease the activation energy required for *CO and C-C coupling.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Fangfang Chang,Juncai Wei,Yongpeng Liu,Wenwen Wang,Lin Yang,Zhengyu Bai
Converting CO 2 to value-added chemicals and fuels by the electrocatalytic reduction reaction (CO 2 RR) is a promising strategy for reducing CO 2 emissions and achieving clean energy storage. Herein, Cu 2 O catalysts with various morphologies (hexapod concave rhombic dodecahedrons microcrystals enclosed with (3 3 1), (1 1 1) and (1 0 0) facets (D-Cu 2 O), cubic microcrystals enclosed with (1 0 0) facet (C-Cu 2 O) and octahedron microcrystals with (1 1 1) and (1 0 0) facets (O-Cu 2 O)) are prepared via the wet chemical reduction method. The in-situ formation of D-Cu 2 O/Cu, C-Cu 2 O/Cu and O-Cu 2 O/Cu surface/interface and the conversion mechanism of CO 2 to C 2+ products have been systematically studied. The electrocatalytic performance of D-Cu 2 O/Cu for CO 2 to form C 2+ products is superior to that of C-Cu 2 O/Cu and O-Cu 2 O/Cu, which the Faraday efficiencies (FE) of C 2+ products (ethylene and ethanol) reaches 70 %. The experimental results combined in-situ Raman spectroscopy and density function theory (DFT) calculations demonstrate that the good electrochemical performance is relate to the surface reconstruction and facet interface, which provides a positive local electronic environment to enhance the adsorption of *CO intermediates and reduces the energy barrier for the activation the C C coupling. This study will provide a new approach to improve the selectivity of CO 2 RR by interface engineering and surface.
研究领域:
材料科学
·
电化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2020
·
IF 5.825
Lijie Zhang,Mei Li,Shengbo Zhang,Xuerui Cao,Jinxiao Bo,Xinli Zhu,Jinyu Han,Qingfeng Ge,Hua Wang
Electrochemical CO 2 reduction (CO 2 RR) to ethanol is a way to advance CO 2 utilization toward a renewable chemical feedstock and fuel. In present study, an approach to promote ethanol production is employed through adding Au, which is favorable toward CO formation, onto Cu 2 O catalysts. Namely, the Cu 2 O hollow nanospheres with a size of 150−180 nm were synthesized by a soft template method, and then Au nanoparticles of ∼7 nm were loaded to obtain Au x /Cu 2 O composites. The Au x /Cu 2 O catalysts have an earlier onset for ethanol production than Cu 2 O. Besides, Au x /Cu 2 O catalysts display the significantly enhanced Faraday efficiencies (FEs) of CO and ethanol, the suppressed hydrogen evolution reaction and the slightly weakened HCOOH formation. Among them, Au 0.17 /Cu 2 O stands out with the highest FEs of ethanol from 10.8%–16.2% throughout the measuring potentials, suggesting an optimal amount of Au. Furthermore, it is found that the FEs of ethanol increase as the atomic ratio of Au/Cu increases at the medium reduction potentials (-1.1 V to -1.3 V). Besides, it is demonstrated that ethanol formation is more favorable over ethylene formation, evidenced by the ratio of FE ethanol /FE ethylene reaching 2.0, 3.3, 4.1 on three Au x /Cu 2 O catalysts, respectively. This correlation between the ethanol production and the Au amount reflects that Au plays a crucial role in promoting ethanol formation. The enhanced ethanol formation is ascribed to more CO formation on Au sites to promote C–C coupling. Our study demonstrates an effective approach to develop Cu-based electrocatalysts for ethanol formation from CO 2 .
研究领域:
化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 10
·2261
·
IF 4.2
Meimei Kou,Ying Yuan,Ruili Zhao,Youkui Wang,Jiamin Zhao,Qing Yuan,Jinsheng Zhao
The insight of the activity phase and reaction mechanism is vital for developing high-performance ammonia synthesis electrocatalysts. In this study, the origin of the electronic-dependent activity for the model Cu2O catalyst toward ammonia electrosynthesis with nitrate was probed. The modulation of the electronic state and oxygen vacancy content of Cu2O was realized by doping with halogen elements (Cl, Br, I). The electrocatalytic experiments showed that the activity of the ammonia production depends strongly on the electronic states in Cu2O. With increased electronic state defects in Cu2O, the ammonia synthesis performance increased first and then decreased. The Cu2O/Br with electronic defects in the middle showed the highest ammonia yield of 11.4 g h−1g−1at −1.0 V (vs. RHE), indicating that the pattern of change in optimal ammonia activity is consistent with the phenomenon of volcano curves in reaction chemistry. This work highlights a promising route for designing NO3−RR to NH3catalysts.
研究领域:
电催化
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Zhenhua Zhang,Liping Fan,Weiqi Liao,Feiyue Zhao,Cen Tang,Jing Zhang,Ming Feng,Ji-Qing Lu
Several CeO 2 -CuO/Cu 2 O nanocomposites with different CuO structures were used to identify the structure sensitivity of CuO in the CeO 2 -CuO/Cu 2 O catalyzed CO oxidation. The CO oxidation catalyzed by various CuO-CeO 2 interfacial sites involves a typical Mars-van Krevelen mechanism, in which the CuO-CeO 2 interfaces in the CeO 2 -CuO/c-Cu 2 O (cubes) nanocomposites are more intrinsically active, exhibiting ca. 15 kJ mol −1 lower activation energy than those in the CeO 2 -CuO/o-Cu 2 O (octahedra) and CeO 2 -CuO/d-Cu 2 O (rhombic dodecahedra) nanocomposites at CeO 2 loadings no less than 0.75 wt%. The higher activity is relevant to lower coordinated oxygen ions on CuO/c-Cu 2 O surface and thus better CO reactivity for the CeO 2 -CuO/c-Cu 2 O nanocomposites, which therefore indicates that the active oxygen species on CuO-CeO 2 interface should come from CuO rather than CeO 2 . Moreover, a highly active 13.2 %CeO 2 -CuO/c-Cu 2 O(s) catalyst for CO oxidation is realized on fine Cu 2 O cubes, which thus has high density of active sites.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 40
·23234-23242
·
IF 12.732
Hongyu Chen,Zhaojie Wang,Shoufu Cao,Siyuan Liu,Xiaojing Lin,Yi Zhang,Yizhu Shang,Qiuying Zhu,Sainan Zhou,Shuxian Wei,Baojun Wei,Daofeng Sun,Xiaoqing Lu
The electrocatalytic CO2 reduction reaction (CO2RR) on copper-based catalysts is a promising method to produce valuable chemicals, but its selectivity is much lower than expected largely due to insufficient research on the structure of new materials. Herein, the antimony-doped Cu/Cu2O (Cu/Cu2O–Sb) catalyst is developed for a highly selective CO2RR to CO. The synthesized Cu/Cu2O–Sb exhibits intensive suppression of hydrogen evolution, a low overpotential and high faradaic efficiency (FE) towards CO. The CO selectivity is as high as ∼95% with a partial current density of ∼6.3 mA cm−2 at −0.9 V and maintains over 90% in a broad range of potentials. DFT calculations reveal that the doping of antimony achieves the distinct activation of CO2 and suppression of hydrogen evolution. Meanwhile, the pre-adsorbed *CO significantly promotes the desorption of the neighboring *CO, which is the key for high selectivity of CO2RR to CO. This work will provide a new consideration for the origin of high selectivity during the CO2RR and pave the way toward design of highly selective CO2 reduction catalysts.
研究领域:
电化学
·
催化
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）