Surfaces and Interfaces
·
2025
·
IF 6.3
Longming Chen,Jun Lu,Tianwei Wang,Caicheng Song,Wenjin Yan,Peng Wang,Chaoran Pang,Yingxin Hu,Rongwen Lu,Shufen Zhang
Nowadays, metal catalysts have great application potential in CO 2 electroreduction reactions, but achieving high current density, high selectivity and good stability in the process of electrolysis remains a major challenge. Herein, a novel nitrogen-doped carbon rods with a chamber structure loaded bismuth (Bi) was firstly synthesized for the electroreduction of CO 2 to formate by a special co-assembly strategy. This strategy features the construction of composite micelles containing metal ions by two surfactants, which is then co-assembled with the melamine-based oligomers constructed based on Schiff base chemistry and yielded the destinated catalyst. Benefiting from the electronic regulation of bismuth by nitrogen species on the support and the confinement effect of chamber structure on metal particles, the as-prepared catalyst shows excellent performance. In a wide potential window, the Faraday efficiency is above 90 %, reaching a maximum of 96 % at -1.3 V vs. RHE, and the partial current density of formate can reach 34.8 mA cm −2 . This work provides a strong candidate for CO 2 electroreduction reactions.
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高影响因子
Surfaces and Interfaces
·
2024
·
IF 5.7
Zhixiu Yang,Xiaoxuan Guo,Yong Chen,Lijing Gao,Ruiping Wei,Guomin Xiao
Modulating the surface microenvironment is crucial in strengthening C C coupling, leading to increasing selectivity in the production of multi-carbon (C 2+ ) products during CO 2 electroreduction. Herein, we have concentrated on investigating how to control the effect of surface distribution of active components of a series of Ag-decorated CuO , denoted as xAg/yCuO. These catalysts with similar chemical elements and morphology are designed, but they exhibit different selectivity in the CO 2 electroreduction process. As a result, the Ag particles in 3Ag/CuO aggregates, while the Ag in 2Ag/2CuO and Ag/3CuO is uniformly distributed on the flower-like CuO nanosphere . Besides, 3Ag/CuO has the highest Faraday efficiency (FE) of CO with a value of 30.9 % at 0.8 V vs. RHE, demonstrating rich-Ag catalysts are beneficial to produce CO. 2Ag/2CuO shows excellent FE C2H4 of 51.4 % at -1.2 V vs. RHE due to the highly dispersed distribution of Ag on the flower-like CuO and higher vacancy O. Ag/3CuO exhibits higher FE H2 compared to other catalysts across a wide potential range, and its minimal impedance is attributed to its exceptional performance in the hydrogen evolution reaction . The proposed reaction pathway for the most effective catalysts 2Ag/2CuO, as determined by in-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS), involves the following steps: CO 2 →*CO 2 − → *COOH → *CO→ *CHO→ *OCHCHO→ *OCHCH 2 → C 2 H 4 . These findings demonstrate that controlling the surface structure can influence the local environment to enhance the efficiency of CO 2 electroreduction.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Shuna Jia,Zhijiang Dong,Zhiqiang Wang,Boxiong Shen,Honghong Lyu
Efficient catalytic reduction of the main greenhouse gas CO 2 into high value-added chemicals is an important measure to alleviate the greenhouse effect and energy depletion. Metal nitrogen (M-N 4 ) macrocyclic complexes have attracted increasing attention in the field of electrocatalytic CO 2 reduction (CO 2 RR) due to the precise adjustment of the catalytic active site according to the requirements and the flexible modification of the external ligand structure. Nevertheless, the poor activity and low selectivity of reduction products restrict their widespread application in electrocatalytic CO 2 RR. Herein, a combination of nanoscale and molecular level method has been developed to construct easily obtainable 4NH 2 -NiPc/NH 2 -CNT hybrid material, in which amino groups are connected to provide electrons toward the central Ni-N 4 site to promote the electrocatalytic CO 2 RR catalytic activity. As a result, the catalyst 4NH 2 -NiPc/NH 2 -CNT mainly produces CO in the electrocatalytic CO 2 RR, which exhibits a Faradaic efficiency of CO (FE CO ) higher than 92 % within a wide overpotential range of −0.70 to −0.95 V vs. RHE, and provides excellent stability with a current density of 12 mA cm −2 at −0.80 V vs. RHE. In addition, 4NH 2 -NiPc/NH 2 -CNT reaches its maximum FE CO value of 96 % at −0.8 V vs. RHE, which is approximately 3.1 times that of the original unmodified NiPc/CNT, demonstrating excellent promotion of electrochemical performance. Similarly, compared to NiPc/CNT without amino modification, the current density of 4NH 2 -NiPc/NH 2 -CNT exceeds it by more than twice. The research results indicate that promoting role of electron substituted amino groups in catalysis dispersion and electronic environment coordination. This study proposes a promising strategy of introducing amino groups into molecular catalysts and hybridizing with carbon nanotube to enhance the electrocatalytic conversion of CO 2 to deep reduction products.
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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高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 40
·23234-23242
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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
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催化
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材料科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Minzhang Li,Man Liang,Wei Wang,Beichi Luo,Yanhong Ji,Longzhang Dong,Lu Guo,Danling Tang,Guangguo Ying,Fuming Chen
Electrochemical desalination offers a promising route to address water scarcity, but current methods often face limitations in salt removal rate and capacity. This study introduces an ultrafast electrocatalytic desalination system that leverages the electrochemical reduction of CO 2 to formate (CO 2 RR) to drive efficient salt removal. The optimized bimetallic Sn/Cu-based polyphthalocyanine (Sn 2 Cu 1 PPc) exhibits exceptional CO 2 RR performance, achieving a peak FE formate of 90.3 % at −1.0 V vs. RHE and a j formate of 84.8 mA cm −2 . In-situ spectroscopic analysis and density functional theory (DFT) calculations reveal that the incorporation of Cu-N 4 units into the Sn-based polyphthalocyanine (SnPPc) promotes CO 2 adsorption and facilitates active hydrogen provision, leading to the observed enhancement in CO 2 RR activity. Using the Sn 2 Cu 1 PPc catalyst, our system achieves a salt removal rate of 1701.3 μg cm −2 min −1 and a formate production rate of 0.79 mmol h −1 cm −2 when treating natural seawater, resulting in potable water with 99.06 % salt removal efficiency. This performance is enabled by a high current density (∼70 mA cm −2 ) during CO 2 RR, which significantly enhances ion transport across the membranes, making this one of the most effective desalination approaches reported. This work demonstrates the potential of coupling CO 2 RR with desalination for sustainable water production and CO 2 mitigation, while also advancing the design of efficient Sn-based electrocatalysts for formate production.
研究领域:
电化学
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环境科学
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材料科学
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能量转换
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水处理
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DOI
高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Shilei Zhang,Hang Wang,Yang Wang,Min Zhang,Weimin Wang,Liang Zhang,Jun Li,Xun Zhu,Qian Fu,Qiang Liao
Elevating the operating pressure could significantly enhance CO2 accessibility on the catalyst in electrochemical CO2 reduction (CO2RR); however, achieving selective production of multi-carbon (C2+) products under pressurized conditions remains a critical challenge because elevated pressure could shift the selectivity towards C1 products. This work systemically investigated the variation of product selectivity induced by pressure and electrolyte composition, and demonstrates that a local pH drop induced by increased pressure is the key reason for hindered C–C coupling, as confirmed by in situ Raman and multi-physics simulation. The elevated pressure results in an increase of the electrolyte's buffering capacity, which neutralizes the alkaline microenvironment near the catalyst, thereby impeding the C–C coupling. Decreasing the buffering ability (using non-buffered KCl electrolyte) or increasing the current density (from 0.4 A cm−2 to 1.0 A cm−2) could maintain a high interfacial alkalinity under elevated pressure, promoting C–C coupling. By mapping pressure–current density operational windows, the optimal conditions were identified, achieving 70% C2 faradaic efficiency (50% for C2H4) at 5 bar and 1 A cm−2, demonstrating superior C2 product selectivity. This work establishes electrolyte engineering principles for industrial CO2RR, enabling carbon-neutral chemical production under practical pressurized conditions through microenvironmental regulation.
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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化学工程
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环境科学
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高影响因子
Energy & Environmental Science
·
2019
·Vol. 12
·期 8
·2455-2462
·
IF 33.25
Zhenglei Yin,Hanqing Peng,Xing Wei,Huan Zhou,Jun Gong,Mingming Huai,Li Xiao,Gongwei Wang,Juntao Lu,Lin Zhuang
The electrochemical conversion of CO2 to fuels or chemicals is an attractive approach that can combine sustainable energy utilization and carbon recycling, but its practicability is still vague, because the CO2 reduction reaction (CO2RR) has hitherto been mostly studied in electrolyte solutions, with small current densities limited by the solubility of CO2. An important and urgent task is thus to develop CO2 electrolyzers that can demonstrate the feasibility of the large-scale conversion of CO2, in particular analogs of water electrolyzers using polymer electrolyte based gas-diffusion electrodes. Here we report a high-performance CO2 electrolyzer making use of alkaline polymer electrolytes (APEs). A highly conductive and stable APE, quaternary ammonia poly(N-methyl-piperidine-co-p-terphenyl) (QAPPT), was applied both as the membrane separator and the ionomer impregnating the gas-diffusion electrodes. Dry CO2 was fed into the Au cathode, with a faradaic efficiency of CO production (COFE) over 85%, and the oxygen evolution reaction (OER) occurred at the IrO2 anode fed with pure water. The cell was operated at temperatures up to 80 °C, and the current density reached 0.5 A cm−2 at 3 V at 60 °C. The stability of this electrolyzer was tested under 0.1 A cm−2, and the cell voltage remained stable at 2.25 V over 100 h, with the COFE staying at 90–95%.
研究领域:
电化学
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可再生能源
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材料科学
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环境工程
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DOI
高影响因子
Energy & Environmental Science
·
2022
·Vol. 15
·期 8
·3494-3502
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IF 39.714
Lianpeng Song,Zhong Liang,Mingzi Sun,Bolong Huang,Yaping Du
The selectivity in the electrocatalysis of carbon dioxide reduction reaction (CO2RR) has attracted tremendous attention but still faces a great challenge. Constructing an interface has become an advanced strategy to effectively modulate electroactivity and selectivity. Herein, we report the synthesis of a CeO2/Bi3NbO7 fibrous tubular structure through a simple electrospinning method, which has shown a much-improved selectivity of 84.73% towards formic acid with remarkable durability in the CO2RR. Theoretical calculations have demonstrated that the construction interface has supplied highly electroactive regions with efficient electron transfer, which not only improves the adsorption of key adsorbates but also alleviates the reaction energy barriers. The modulation induced by the interface enables the high selectivity and yield of HCOOH. This work has supplied a novel and advanced strategy to utilize the interfacial effect in developing superior CO2RR electrocatalysts in the future.
研究领域:
材料科学
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电化学
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催化
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环境科学
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DOI
高影响因子
Nature Communications
·
2021
·Vol. 12
·期 1
·1-11
·
IF 14.919
Sun Hao,Chen Ling,Xiong Likun,Feng Kun,Chen Yufeng,Zhang Xiang,Yuan Xuzhou,Yang Baiyu,Deng Zhao,Liu Yu,Rümmeli Mark H.,Zhong Jun,Jiao Yan,Peng Yang
Electrochemical CO 2 reduction (CO 2 RR) in a product-orientated and energy-efficient manner relies on rational catalyst design guided by mechanistic understandings. In this study, the effect of conducting support on the CO 2 RR behaviors of semi-conductive metal-organic framework (MOF) — Cu 3 (HITP) 2 are carefully investigated. Compared to the stand-alone MOF, adding Ketjen Black greatly promotes C 2 H 4 production with a stabilized Faradaic efficiency between 60-70% in a wide potential range and prolonged period. Multicrystalline Cu nano-crystallites in the reconstructed MOF are induced and stabilized by the conducting support via current shock and charge delocalization, which is analogous to the mechanism of dendrite prevention through conductive scaffolds in metal ion batteries. Density functional theory calculations elucidate that the contained multi-facets and rich grain boundaries promote C–C coupling while suppressing HER. This study underlines the key role of substrate-catalyst interaction, and the regulation of Cu crystalline states via conditioning the charge transport, in steering the CO 2 RR pathway.
研究领域:
电化学
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材料科学
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催化
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能源转换
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 20
·10892-10901
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IF 14.511
Wenfei Dong,Nan Zhang,Sanxiu Li,Shixiong Min,Juan Peng,Wanyi Liu,Dongping Zhan,Hongcun Bai
The electrocatalytic reduction of CO2 using electricity produced from renewable resources is a strategy for achieving CO2 emission reduction and sustainable energy development. Further, the reaction has a large number of industrial practical applications, since CO2 can be converted to fuels via downstream chemical processing of the CO product. Herein, we successfully synthesized a low Mn-content single-atom catalyst (SAC) with Mn–N2O2 sites, covalently integrated into carbon nanosheets (Mn–NO/CNs) using a one-pot synthesis method. The Mn–NO/CN catalyst displays efficient electrocatalytic performance for the CO2 reduction reaction (CO2RR). Using an H-type electrolytic cell, the maximum CO Faraday efficiency (FE) at −0.460 V (V vs. RHE) reaches 96.0% in 0.5 M KHCO3 electrolyte. In the flow cell measurements, Mn–NO/CNs exhibits a current density of 28 mA cm−2 at a very low potential of −0.425 V (V vs. RHE) for the CO2RR with 1.0 M KOH as the mobile phase. The FECO remains above 80% even after 70 h, demonstrating the excellent durability of the catalyst even at a very low potential. The X-ray absorption spectra (XAS) and DFT calculations show that the Mn–N2O2 site is the active catalytic center, which facilitates the adsorption of CO2 and significantly lowers the free energy barrier leading to the formation of the critical intermediate *COOH. The presence of dual N and O coordinated to the single atom metal sites embedded in the 2D carbon nanosheet significantly improves catalytic activity for the reduction of CO2. Therefore, the catalytic performance of the single atom metal catalyst can be enhanced by adjusting the coordination environment.
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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环境科学
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DOI
高影响因子
Inorganic Chemistry Frontiers
·
2018
·Vol. 5
·期 7
·1524-1532
·
IF 5.106
Jun-Hao Zhou,Da-Wei Lan,Sheng-Song Yang,Yu Guo,Kun Yuan,Lin-Xiu Dai,Ya-Wen Zhang
Bimetallic hollow structures can be efficiently used to improve the utilization of noble metals in electrocatalysts, but few studies have reported the application of bimetallic hollow nanocomposites for the electrochemical reduction of CO2. Herein, we demonstrated the synthesis of hollow Au–Cu nanoparticles of size ranging from 50 nm to 100 nm with a wall thickness of 4.95 ± 0.81 nm for efficient CO2 reduction reaction (CO2RR) via galvanic replacement and the Kirkendall effect between copper and gold. In the fabrication procedure, a gold precursor was pre-dissolved in TOP to lower the reduction potential of Au3+, which could then be reduced by Cu0. The obtained hollow Au–Cu NPs were then supported on carbon black for CO2RR measurement, and it exhibited a maximum CO FE of 53.3% at −0.7 V (vs. RHE), which was very close to that of Au NP/C, but the gold mass current density of hollow Au–Cu NP/C was much higher. The hollow Au–Cu NP/C also showed good stability in long-time measurements for CO2RR. To find out how the superior catalytic performance was achieved, hollow Au–Cu NP/C was then annealed in O2 and N2. It was found that after being annealed, the catalysts almost totally lost the activity towards CO2RR, which may be due to the partial segregation of Cu species on the nanoparticle surface as well as a decrease in the surface defect density with the improvement in crystallinity. Thus, it was concluded that high dispersion of more Au atoms on the nanoparticle surface together with the presence of more surface defect sites could account for the superior CO2RR performance of the as-synthesized hollow Au–Cu NP/C.
研究领域:
材料科学
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电化学
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纳米技术
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催化
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Yahui Jiang,Haichuan He,Dan Xia,Hongwei Zhang,Shirui Tan,Li Luo,Yifan Kong,Liu Deng,You-Nian Liu
Cu-based catalysts are widely employed in the electrocatalytic CO2 reduction reaction (CO2RR) toward multi-carbon (C2+) products due to their unique electronic structures. However, Cu-based catalysts are prone to reconstruction under working conditions. Self-reduction and undesirable reconstruction have limited the activity and selectivity of these catalysts. Understanding their reconstruction behavior is crucial for elucidating reaction mechanisms and rationally designing catalysts. In this study, Br-doped Cu-base catalysts were employed to investigate the influence of dopants on catalyst surface reconstruction during CO2RR. Characterizations confirmed that during CO2RR, partial Br− leached from the precursor, while residual bromide ions in the Cu matrix created a bromine-rich environment on the catalyst surface, stabilizing Cu0/Cu+ active sites. The reconstructed catalyst exhibited superior selectivity for C2+ products and higher current density. In situ characterization and theoretical calculations demonstrated that the interaction between Br and Cu atoms suppressed complete Cu reduction. Furthermore, the asymmetric coupling pathway via *CO and *CHO intermediates dominated C2+ product formation, with significantly reduced Gibbs free energy of key intermediates compared to undoped CuO. Notably, halogen doping was validated as a universal strategy—Cu–Cl and Cu–F catalysts similarly enhanced C2+ production while exhibiting analogous reconstruction behavior. This study provided deep insights into catalyst surface reconstruction and offered effective strategies for designing high-performance catalysts for CO2RR.
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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环境化学
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能量转换
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表面科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）