ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Zhijian Chen,Zhenghui Ma,Guoli Fan,Feng Li
Presently, realizing high ethanol selectivity in CO2 electroreduction remains challenging due to difficult C–C coupling and fierce product competition. In this work, we report an innovative approach for improving the efficiency of Cu-based electrocatalysts in ethanol generation from electrocatalytic CO2 reduction using a crystal plane modification strategy. These novel Cu-based electrocatalysts were fabricated by electrochemically activating three-dimensional (3D) flower-like CuO micro/nanostructures grown in situ on copper foils and modifying with surfactants. It was demonstrated that the fabricated Cu-based electrocatalyst featured a predominantly exposed Cu(100) surface loaded with high-density Cu nanoparticles (NPs). The optimal Cu-based electrocatalyst displayed considerably improved CO2 electroreduction performance, with a Faraday efficiency of 37.9% for ethanol and a maximum Faraday efficiency of 68.0% for C2+ products at −1.4 V vs RHE in an H-cell, accompanied by a high current density of 69.9 mA·cm–2, much better than the particulate Cu-based electrocatalyst. It was unveiled that the Cu(100)-rich surface of nanoscale petals with abundant under-coordinated copper atoms from CuNPs was conducive to the formation and stabilization of key *CH3CHO and *OC2H5 intermediates, thereby promoting ethanol generation. This study highlighted the critical role of CuNP-loaded Cu(100) surface structures on structured Cu-based electrocatalysts in enhancing ethanol production for the CO2 electroreduction process.
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
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Xianlong Lu,Lili Wang,Xueyang Zhao,Binbin Pan,Zhendong Li,Xiangfei Du,Shihan Zhang,Fan Dong,Bangwei Deng
Copper (Cu)-based catalysts show significant potential for producing high value-added C 2+ products in electrocatalytic CO 2 /CO reduction reactions (CO (2) RR). However, the structural reconfiguration during operation poses substantial challenges in identifying the intrinsic catalytic active site, especially under similar mass transport conditions. Herein, three typical and commercial Cu-based catalysts (Cu, CuO, and Cu 2 O) are chosen as representatives to elucidate the structure-activity relationship of CORR in the membrane electrode assembly electrolyzer. Notably, only the Cu catalyst demonstrates the most suppression of hydrogen evolution reaction, thus achieving the highest FE of 86.7% for C 2+ products at a current density of 500 mA cm –2 and maintaining a stable electrolysis over 110 h at a current of 200 mA cm –2 . The influence of chemical valence state of Cu, electrochemical surface area, and local pH were firstly investigated and ruled out for the significant FE differences. Finally, based on the structure analysis from high resolution transmission electron microscope, OH – adsorption, in situ infrared spectroscopy and density functional theory calculations, it is suggested that the asymmetric C-C coupling ( via *CHO and *CO) is the most probable reaction pathway for forming C 2+ products, with Cu (100)-dominant grain boundaries (GBs) being the most favorable active sites. These findings provide deeper insights into the synergistic relationship between crystal facets and GBs in electrocatalytic systems.
研究领域:
电化学
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催化
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材料科学
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纳米技术
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Lili Gao,Langlang Qin,Haonan Wu,Xuelian Li,Kai Qi,Qun Yi,Jiandong Zhang,Lijuan Shi
Electrochemical reduction of CO 2 (CO 2 ER) to high value-added multicarbon (C 2+ ) is a viable way to promote carbon–neutral cycle. To date, copper (Cu) is reported as the most effective metal catalyst toward C 2+ , but it remains a challenge to achieve high selectivity and large current density. Incorporating ionic liquid in Cu-based catalysis has been proved an effective strategy, however, most reported methods are either involved too much ionic liquid (IL) as electrolyte or too complex & unstable. Herein, an ionic liquid-embedded Cu electrocatalyst (Cu-IL/GDL) was innovatively constructed through one-step electro-codeposition method, in which a kind of amino-ionic liquid, AFIL, was anchored to the gas diffusion layer (GDL) and embedded by the deposited Cu. Under the excellent synergy between Cu and AFIL, Cu-IL/GDL exhibits higher faradaic efficiency toward ethylene (C 2 H 4, 40.67%) and C 2 (C 2 H 4 and C 2 H 5 OH, 61.39%) when directing CO 2 to carbon-fiber side of electrode in H-cell. To be precise, more Cu (1 0 0) facet is stabilized by the capping effect of AFIL, being in favor for C–C coupling; meanwhile more AFIL + is embedded by the deposited Cu, making for the initiation of CO 2 ER. Thus, this paper proposes a facial and effective strategy to reinforce Cu (1 0 0) facet, and couple and heighten the virtues of ionic liquid and Cu during CO 2 ER toward C 2 .
研究领域:
化学
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材料科学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2024
·Vol. 16
·期 6
·3034-3042
·
IF 5.8
Haoyang Wu,Zhili Wang,Benqiang Tian,Yaping Li,Zheng Chang,Yun Kuang,Xiaoming Sun
Electrocatalytic CO2 reduction (ECR) to high value-added chemicals is an excellent method to attenuate the impact of greenhouse effect caused by CO2. At the same time, multicarbon products (C2+) get extensive attention in view of their relatively high energy density and market price. At present, Cu is an important metal electrocatalyst to convert CO2 into multicarbon products (e.g. ethylene, ethanol, and n-propanol); however, its poor selectivity impedes its practical application. It is well-known that the Cu(100) crystal facet can enhance the selectivity toward multicarbon products among different Cu crystal facets. Herein, the Cu nanoparticles were firstly prepared using the inductive effect of different gases (CO2, CO, Ar, N2, and air) during the Cu electrodeposition processes, in which the CO2-induced Cu catalyst (Cu-CO2) showed the largest normalized content of the Cu(100) crystal facet and the highest C2+ faradaic efficiency of 69% at a current density of 80 mA cm−2 in ECR. Subsequently, the different CO2 pressures during the Cu electrodepositions were studied to reveal the optimal CO2 pressure in the CO2-induced Cu synthesis for improved Cu(100) content as well as C2+ faradaic efficiency. Finally, density functional theory (DFT) calculations confirmed that CO2 molecules preferred to get adsorbed on the Cu(100) crystal facet, which resulted in not only the presence of dominant Cu(100) during the CO2-induced Cu synthesis but also the good electrocatalytic performance in ECR.
研究领域:
材料科学
·
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Nanotechnology
·
2020
·Vol. 15
·期 10
·848-853
·
IF 31.538
Jiang Lizhi,Liu Kunlong,Hung Sung-Fu,Zhou Lingyun,Qin Ruixuan,Zhang Qinghua,Liu Pengxin,Gu Lin,Chen Hao Ming,Fu Gang,Zheng Nanfeng
Hydrogen spillover is a well-known phenomenon in heterogeneous catalysis; it involves H 2 cleavage on an active metal followed by the migration of dissociated H species over an ‘inert’ support 1 , 2 , 3 , 4 , 5 . Although catalytic hydrogenation using the spilled H species, namely, spillover hydrogenation, has long been proposed, very limited knowledge has been obtained about what kind of support structure is required to achieve spillover hydrogenation 1 , 5 . By dispersing Pd atoms onto Cu nanomaterials with different exposed facets, Cu(111) and Cu(100), we demonstrate in this work that while the hydrogen spillover from Pd to Cu is facet independent, the spillover hydrogenation only occurs on Pd 1 /Cu(100), where the hydrogen atoms spilled from Pd are readily utilized for the semi-hydrogenation of alkynes. This work thus helps to create an effective method for fabricating cost-effective nanocatalysts with an extremely low Pd loading, at the level of 50 ppm, toward the semi-hydrogenation of a broad range of alkynes with extremely high activity and selectivity.
研究领域:
催化
·
材料科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
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