Journal of Energy Chemistry
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2024
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IF 14
Haotian Duan,Wenyang Li,Lixiu Ran,Fulong Zhu,Tianxiang Li,Ming Miao,Wen-jin Yin,Xin Wang,Yongzhu Fu
The conversion of carbon dioxide to ethylene by electrochemical reduction (CO 2 RR) provides a new strategy for achieving carbon dioxide conversion. However, copper-based catalysts have the disadvantages of unsatisfactory selectivity and low current density, which limit the potential CO 2 RR industrial expansion. Researches have verified that the real reaction sites at the catalyst surface often undergo reconstruction during the reaction, therefore, understanding and utilizing this phenomenon is crucial for improving catalytic performance. In this work, we introduced additional Ag component into Cu@Ag/C tandem catalyst by in-situ electrochemical reconstruction of Cu 2 CO 3 (OH) 2 /AgCl/C precursor. This electro-reduced catalyst exhibits a C 2 H 4 Faradaic efficiency of 50.41% in H-cell, and 58.03% in the flow cell, surpassing the counterparts of pure Cu and Ag, as well as the Cu-Ag homolog with separated interface. Moreover, it also provides a long-term stability of 21 h with the ethylene Faraday efficiency (FE) over 50%. The appropriate amount of Ag dopant into the Cu catalyst changes the electronic structure of Cu surface by the electron transfer from Cu to Ag, which distinctly enhances the binding energy of CO 2 on the catalyst. Meanwhile, in-situ Raman results and theoretical calculation reveal that the introduction of silver increases the number of active sites and improves the coverage of *CO intermediate, thereby accelerating the kinetics of C–C coupling and reducing its energy barrier. The combination of cascade catalytic strategy and in-situ electroreduction interface provides potential applications for future artificial carbon balance.
研究领域:
材料科学
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电化学
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催化反应
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产品关联
DOI
高影响因子
ULTRASONICS SONOCHEMISTRY
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2021
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IF 7.491
Yang Yang,Yiqing Feng,Kejian Li,Saira Ajmal,Hanyun Cheng,Kedong Gong,Liwu Zhang
Among the possible products of CO 2 electrochemical reduction, CO plays a unique and vital role, which can be an ideal feedstock for further reduction to C 2+ products, and also the important component of syngas that can be used as feedstock for value-added chemicals and fuels. However, it is still a challenge to tune the CO selectivity on Cu electrode. Here we newly construct an ultrasound-assisted electrochemical method for CO 2 reduction, which can tune the selectivity of CO 2 to CO from less than 10% to >80% at −1.18 V versus (vs.) reversible hydrogen electrode (RHE). The partial current density of CO production is significantly improved by 15 times. By in-situ Raman study, the dominating factor for the improved CO production is attributed to the accelerated desorption of *CO intermediate. This work provides a facile method to tune the product selectivity in CO 2 electrochemical reduction.
研究领域:
电化学
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材料科学
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DOI
高影响因子
ELECTROCHIMICA ACTA
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2021
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IF 6.901
Bao Liu,Chao Cai,Baopeng Yang,Kejun Chen,Yan Long,Qiyou Wang,Shuandi Wang,Guozhu Chen,Hongmei Li,Junhua Hu,Junwei Fu,Min Liu
Electrochemical carbon dioxide (CO 2 ) reduction reaction (CO 2 RR) to obtain C2/multi-carbon fuels is an appealing technology to reduce carbon emission and store intermittent renewable electricity. The C–C coupling process, as the most critical step for generating C2/multi-carbon fuels, strongly depends on the concentration of *CO intermediates around the active sites. In this work, we prepared porous copper nanospheres (P-Cu) that greatly improved the C–C coupling process by enriching *CO intermediates in the pore structure . The specific pore features of P-Cu were characterized in detail by scanning electron microscopy (SEM), transmission electron microscopy (TEM), and nitrogen adsorption/desorption tests. Obviously, the P-Cu exhibits higher specific surface area and richer pore structure than the control sample compact copper nanosphere (C-Cu). The CO gas sensor and temperature programmed desorption (TPD) tests prove that the P-Cu has better CO adsorption and enrichment capacity than C-Cu due to the rich pore structure. As a result, P-Cu exhibited a high C2 selectivity with a Faradaic efficiency (FE C2 ) of 57.22% at −1.3 V ( vs . RHE), which is about 2.5-fold than the C-Cu (FE C2 of 22.71%). This work provides an effective strategy to improve the activity and selectivity of C2 products in CO 2 RR by optimizing the adsorption/enrichment property of intermediates.
研究领域:
材料科学
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能源化学
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催化化学
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DOI
高影响因子
Green Energy & Environment
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2024
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IF 10.7
Junming Zeng,Yongbin Yao,Fang Wang,Jiajian Gao,Lili Zhang,Guangwen Xu,Ziyi Zhong,Fabing Su
Nickle-based catalysts are commonly used for CO 2 methanation. However, there is still potential to improve their catalytic performance under mild conditions. In this study, we synthesized a series of Ru-Ni-Al catalysts from Ru-doped NiAl-hydrotalcite using a hydrothermal method. The Ru-Ni-Al catalyst demonstrated much higher activity for CO 2 methanation than the Ni-Al catalyst that did not have Ru doping. Both experimental results and theoretical calculations indicate that the enhanced performance of the Ru-Ni-Al catalyst is related to electronic interactions between nickel (Ni) and ruthenium (Ru). The Ru sites transfer electrons to the Ni sites, increasing the local electron density of Ni, which enhances the adsorption and activation of H 2 . Furthermore, the Ru-Ni metal interface sites improve the adsorption and activation of CO 2 . In situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis indicates that adjusting the electronic structure of Ni sites can accelerate the production of intermediates HCOO*, while Ru-Ni intermetallic interface sites can directly dissociate CO 2 into CO*. In addition, CO 2 methanation on the Ru-Ni-Al catalyst follows HCOO*- and CO*-mediated pathways. This study underscores the potential for enhancing CO 2 methanation performance by modulating the electronic structure of Ni sites.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Kai Zhu,Zihan Lin,Xinyi Bai,Fangfang Chang,Qing Zhang,Xiaolei Wang,Zhengyu Bai
Electrocatalytic reduction reaction of CO2 (CO2RR) into value-added multicarbon (C2+) products represents a sustainable strategy for mitigating greenhouse gas emissions and enhancing the production of high-value chemicals. Cu-based catalysts are optimal for the CO2RR, facilitating the generation of C2+ products such as ethanol, which have significant industrial applications. However, converting CO2 to C2+ products remains a great challenge, necessitating the simultaneous achievement of high current density, Faradaic efficiency (FE), and operational stability for industrial-scale implementation. Herein, we prepared Cu/Cu2O catalysts with diverse morphologies and the ratio of the Cu+/Cu interface, which was rectified by regulating the interactions between the active interface and the intermediate (*CO). The electrochemical analysis demonstrated that reconstructed Cu/Cu2O nanodendrites with dominant grain boundaries exhibited remarkable performance in generating C2+ products, achieving a Faradaic efficiency (FE) of 71.8%, including 49.7% FE of ethanol and a substantial partial current density of 390.0 mA cm–2 within the flow cell. In situ spectroscopy characterization and theoretical calculations revealed that the increased ethanol selectivity originated from the rectification of the Cu/Cu2O interface by the *CO intermediate, which accelerated H2O dissociation, reduced the free energy for *CO hydrogenation to *COH, and facilitated asymmetric *CO-*COH coupling to preferentially reduce CO2 to ethanol. This study provides profound insights into the C–C coupling pathways and sheds light on the rational design of ethanol-oriented electrocatalysts, contributing to sustainable chemical synthesis and energy utilization.
研究领域:
电催化
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能量转换
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材料科学
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环境化学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Rui Hua,Jiale Zhao,Houde She,Lei Wang,Jingwei Huang,Qizhao Wang
Copper serves as an exceptional cocatalyst, enhancing CO 2 molecular adsorption-activation and stabilizing reaction intermediates, thus demonstrating remarkable potential in photocatalytic CO 2 conversion to diverse hydrocarbons. However, the complex and variable oxidation states of Cu make the role and mechanism of low-valent Cu species (Cu 0 /Cu + ) in CO 2 photoreduction poorly understood. This study precisely controlled the valence distribution of Cu species on TiO 2 surfaces using a red phosphorus-mediated hydrothermal synthesis strategy, successfully constructing an efficient catalyst for CO 2 photoreduction. The optimized composite exhibits a CH 4 evolution rate of 64.44 μmol·g −1 ·h −1 under simulated sunlight, representing a 54-fold improvement over pristine TiO 2 while maintaining high selectivity of 86 %. The enhanced photocatalytic performance and product selectivity originate from Cu incorporation, which substantially improves light absorption capacity, prolongs charge carrier lifetime, and reduces charge transfer resistance. Combined characterization and DFT calculations conclusively demonstrate that Cu 0 and Cu + serve as the active sites for CH 4 and CO generation, respectively. The key intermediate *CO preferentially desorbs as CO from Cu + sites, while *CO adsorbed on Cu 0 sites undergoes further hydrogenation to form CH 4 . This work provides novel strategies for developing efficient CO 2 photoreduction catalysts and elucidates the atomic-scale mechanistic role of Cu valence states in regulating CO 2 reduction pathways.
研究领域:
催化
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材料科学
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环境科学
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物理化学
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）