AICHE JOURNAL
·
2023
·Vol. 69
·期 10
·e18161
·
IF 3.7
Zhanshuai Ma,Tianyu Zhang,Lili Lin,Aijuan Han,Junfeng Liu
Developing highly active, selective, and stable electrocatalysts for the CO 2 reduction reaction (CO 2 RR) is essential to relieve the greenhouse effect and the energy crisis. Traditional catalytic electrodes require ionomer binders, which inevitably impose undesired high CO 2 transport resistance and block the active sites. Herein, Ni single atoms anchored on nitrogen-doped carbon nanoarrays (denoted as Ni-SAC-NA) were developed as the electrode without additional ionomers for efficient CO 2 RR. The unique nanoarray structure provided a higher specific surface area, more exposed active sites, and enhanced electron/mass transport due to its short diffusion pathway and ionomer-free nature. As a result, the Ni-SAC-NA electrode exhibited enhanced activity of CO 2 RR and selectivity towards CO with Faradaic efficiency of 96.7%, turnover frequency of 27,504 h −1 , and cathodic energy efficiencies of 54.9% at −0.88 V (vs. RHE). Our findings provide a rational design strategy for CO 2 RR electrocatalysts by constructing ionomer-free electrodes.
研究领域:
材料科学
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能源化学
·
环境科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Yanzhi Xu,Changli Li,Yequan Xiao,Chenghui Wu,Yanming Li,Yanbo Li,Juguang Han,Qinghua Liu,Jingfu He
The combination of Cu and Ag presents a promising way to steer the CO2 reduction products through regulating the surface active sites. However, the difficulty in forming the CuAg alloy with a controllable atomic ratio impedes the in-depth understanding of the structure–activity relationship of CuAg catalysts. Herein, we use E-beam evaporation to synthesize a series of CuAg films with uniform distribution and controllable stoichiometry to reveal the real reaction mechanism on CuAg for the electrochemical CO2 reduction process. Compared with Cu, the Cu1–xAgx (x = 0.05–0.2) alloy showed an apparent suppression of HCOOH and the ratio between C2 liquid products (e.g., ethanol and acetate) and C1 liquid product (HCOOH) is also increased. Operando synchrotron radiation Fourier transform infrared spectroscopy results suggest that the introduction of Ag into the Cu phase can significantly strengthen the absorbed *CO and *OCCO intermediates and suppress the O–C–O intermediates. This research provides a reliable way to inhibit the generation of HCOOH and enhance the production of liquid C2 products during CO2RR and presents a guideline for the future manipulation of copper catalysts by alloying.
研究领域:
材料科学
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催化化学
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DOI
PubMed
高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Xianda Zhang,Yaotian Yan,Yangshuo Liu,Chun Li,Jian Cao,Junlei Qi
CO2 reduction reaction (CO2RR) has been considered as a promising process that can compensate CO2 emission and convert it into value-added chemicals. In preparation of CO2RR catalytic electrode, Nafion is a common binder but its effect in catalytic process is usually ignored. Herein, we proposed the bifunction of Nafion in CO2RR based on its molecular structure and successfully developed a CO2-affinitive surface of Micro-Ag /Nafion by controlling the content of Nafion, which exhibited a superior CO faradaic efficiency (FECO) of 95.07% at -0.9 V (vs. RHE). This excellent FECO and 2 times of CO partial current density (jCO) in flow-cell proved its industrial prospect. Its splendid selectivity of CO2RR was attributed to the selective polarization of CO2 molecule at Nafion, which resulted in the 6.8 times higher adsorption energy (Eads) of CO2 than H2O. Therefore, CO2RR gained an advantage in the competitive reaction.Nafion was recognized as a favorable transporter for CO2 on the surface of metal catalyst. Our work describes the bifunctional role of Nafion in CO2RR electrode and it will contribute to optimize the design of metal/Nafion catalytic material for CO2RR.
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高影响因子
Nano Energy
·
2026
·
IF 16.7
Rui Li,Xupeng Qin,Yang Liu,Shen Cheng,Haixin Sun,Qizheng An,Youcai Che,Jingqiu Shang,Xin Chen,Shuowen Bo,Junfeng Yang,Qinghua Liu
P-modulated Fe single atoms are designed to steer interfacial PCET pathways. • Remote P-doping reconfigures interfacial water networks for optimal proton supply. • In situ spectra and simulations reveal accelerated *COOH formation kinetics. • The FeNPC catalyst achieves a remarkable CO Faradaic efficiency of 98.68%. In electrocatalytic CO₂ reduction reaction (CO₂RR), the rate-determining formation of the key *COOH intermediate requires a facile and moderate proton supply, yet excessive water activation generates abundant adsorbed hydrogen (*H) that triggers the competing hydrogen evolution reaction (HER) and diminishes CO selectivity. Here, we develop a phosphorus-doped Fe single-atom catalyst (FeNPC) to steer interfacial proton-coupled electron transfer (PCET) pathways. P incorporation reconstructs the interfacial hydrogen-bonding network, selectively enriching weakly hydrogen-bonded and free water molecules to ensure an optimal proton supply for *COOH generation while suppressing excessive *H accumulation. In-situ ATR-SEIRAS characterization confirms enhanced *COOH signals, and MD/DFT calculations reveal that P-doping lowers activation barriers for water dissociation and *COOH formation. Consequently, FeNPC achieves a CO Faradaic efficiency of 98.68% at −0.4 V vs. RHE with reliable stability. This work demonstrates that nonmetallic doping optimizes PCET kinetics by reshaping the interfacial water microenvironment, establishing a new paradigm for designing highly-selective CO₂RR electrocatalysts. Download: Download high-res image (273KB) Download: Download full-size image
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高影响因子
DALTON TRANSACTIONS
·
2025
·Vol. 54
·期 23
·9160-9168
·
IF 3.3
Jiansheng Ye,Yali Dai,Wenjun Liu,Jingrou Xu,Jialing Li,Meng Chen,Sha Yang,Qinzhen Li,Yuanxin Du,Jinsong Chai,Manzhou Zhu
Taking Au36(CHT)24 (Au36 for short) as a precursor, a Au32(CHT)20(TFP) (Au32 for short) nanocluster is obtained with the aid of a phosphine-mediated approach. Structural analysis shows that Au32 is obtained by modifying and transforming the surface structure of the parent Au36 nanocluster, including the removal of a surface layer of the core structure and the rearrangement of the surface motifs. Most importantly, this structural transformation results in a change in the position of some of the surface motifs, thus exposing the active domain with bare core metal atoms. The electrocatalytic CO2 reduction reaction is introduced to investigate the effect of the modification of the surface structure on its properties. The results show that the modified structure of Au32 exhibits superior catalytic activity with a faradaic efficiency (for CO) of 97.7% at −0.8 V.
研究领域:
材料科学
·
电化学
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产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Haojun Shi,Lingli Luo,Congcong Li,Yu Li,Tingting Zhang,Zhongliang Liu,Jialin Cui,Li Gu,Ling Zhang,Yanjie Hu,Huihui Li,Chunzhong Li
Copper oxide nanomaterials have been suggested to be efficient for highly selective multi-carbon (C 2+ ) production in CO 2 reduction reaction (CO 2 RR), due to the introduction of surface Cu + species from oxide catalysts. However, the Cu + species on the catalyst surface are prone to being reduced to Cu 0 under reductive conditions during CO 2 RR. Here, a network-structured catalyst is developed consisting of ultrafine Cu 2 O/CuO nanoparticles that harbor an abundance of pores. This catalyst is synthesized via flame spray pyrolysis (FSP) method and engineered to confine carbon intermediates, which subsequently cover the local catalyst surface and stabilize Cu + species. As a result, a C 2+ products Faradaic efficiency (FE) of approximately 80.0% at a partial current density of 320.0 mA cm −2 is achieved, and a large C 2+ to C 1 ratio of ≈9.7. In situ XRD and XPS spectra are employed to reveal the indeed presence of Cu + species on the catalyst surface during the CO 2 RR process, which extensively improves the adsorption of * CO intermediates and thus the C─C coupling reaction to form C 2+ products.
研究领域:
催化
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材料科学
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电化学
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可持续能源
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产品关联
DOI
高影响因子
LANGMUIR
·
2026
·
IF 4.4
Honglin Li,Yingqi Duan,Qingwen Feng,Linjiao Wei,Jingbin Zeng,Ziyue Chen,Qingtong Zhang,Yanpeng Chen,Zifeng Yan
Ag–Cu tandem catalysis provides an effective strategy to enhance C2+ selectivity in the electrochemical CO2 reduction reaction (CO2RR) by integrating CO generation and utilization for C–C coupling. Here, we report a series of Ag@Cu2O, Ag@CuO, and Ag@CuO-BDC core–shell catalysts designed to regulate the CO generation, Cu-oxidation states, and surface structures. The Ag@Cu2O catalysts exhibit pronounced tandem effects, suppressing CH4 formation while enhancing the C–C coupling on the Cu sites. Notably, Ag@Cu2O-30 achieves a high C2H4/CH4 Faradaic efficiency ratio of 6.5 at −1.8 V (vs RHE) with an increased C2H4 partial current density of 12.3 mA cm–2. Oxidation to Ag@CuO further modifies the Cu species distribution, facilitating CO and CO2 diffusion while reducing H2 formation. Moreover, constructing Cu-BDC-MOF followed by electrochemical reconstruction generates additional oxygen vacancies and stabilizes Cu+ species, enhancing C2H4 selectivity and stability but with increased CH4 formation and reduced current density. This study highlights Ag–Cu tandem catalysis and structural regulation of Cu as effective strategies for achieving selective reduction of CO2 toward C2H4.
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DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
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2026
·
IF 4.6
Jialuo Li,Guojie Gao,Yu Wei,Taolue Liu,Hanwen Xu,Mingxia Guo,Xin Ding,Yan Gao
Abstract Coupling CO2 reduction with thermodynamically favorable anodic oxidation offers a promising route for lowering the energy demand of paired electrosynthesis. Herein, we report a bismuth-based paired electrosynthesis system (Bi NSs/CF || Bi/NF-20) for the simultaneous coproduction of high value formate at both electrodes via cathodic CO2 reduction (CO2RR) and anodic methanol oxidation (MOR). Crucially, these self-supported electrodes are rationally constructed through a spontaneous galvanic replacement strategy, offering a sustainable alternative to conventional energy intensive fabrication. Consequently, the integrated two-electrode electrolyzer operates stably at 3 V for 50 h, yielding a combined FE exceeding 185% and impressive production capacities of more than 400 g kWh–1. Combined in situ Raman spectroscopy and theoretical calculations reveal that the intrinsic electronic properties of the Bi NSs/CF facilitate the rate-determining step by lowering the *OCHO formation barrier, and elucidate the dynamic evolution of active sites during the MOR. This study offers a compelling strategy for designing integrated electrolyzers toward CO2 valorization with high atom economy.
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高影响因子
Nanomaterials
·
2023
·Vol. 13
·期 11
·1767
·
IF 5.3
Wenqin Lai,Yating Liu,Mingming Zeng,Dongmei Han,Min Xiao,Shuanjin Wang,Shan Ren,Yuezhong Meng
The rapid development of electrochemical CO2reduction offers a promising route to convert intermittent renewable energy into products of high value-added fuels or chemical feedstocks. However, low faradaic efficiency, low current density, and a narrow potential range still limit the large-scale application of CO2RR electrocatalysts. Herein, monolith 3D bi-continuous nanoporous bismuth (np-Bi) electrodes are fabricated via a simple one-step electrochemical dealloying strategy from Pb-Bi binary alloy. The unique bi-continuous porous structure ensures highly effective charge transfer; meanwhile, the controllable millimeter-sized geometric porous structure enables easy catalyst adjustment to expose highly suitable surface curvatures with abundant reactive sites. This results in a high selectivity of 92.6% and superior potential window (400 mV, selectivity > 88%) for the electrochemical reduction of carbon dioxide to formate. Our scalable strategy provides a feasible pathway for mass-producing high-performance and versatile CO2electrocatalysts.
研究领域:
材料科学
·
电化学
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产品关联
DOI
PubMed
高影响因子
ChemSusChem
·
2026
·Vol. 19
·期 10
·e70648
·
IF 5.9
Yunjia Yang,Jingjing Wang,Xinli Shi,Jingqian Zhang,Pengfei Yin,Boxiong Shen,Lang Jiang
Zinc (Zn) is an attractive electrocatalyst for converting CO 2 to carbon monoxide (CO) via the carbon dioxide reduction reaction (CO 2 RR), but its application is limited by poor selectivity and stability. In contrast to conventional crystalline modifiers or bulk buffers, we report a bifunctional strategy using an amorphous phosphate layer to simultaneously enhance proton transfer and stabilize Zn active sites. Amorphous phosphate-modified zinc nanoflakes (Zn-HPO 4 NF) were synthesized through a simple two-step method. At −1.3 V versus RHE, the Zn-HPO 4 catalyst delivers a CO Faradaic efficiency (FE CO ) of 86.4%. The catalyst exhibits exceptional durability at −1.4V versus RHE, sustaining a stable current of ~17 mA over 20 h with an average FE CO exceeding 80% and negligible current decay, significantly outperforming pure Zn. In situ spectroscopy and operando electrochemical impedance spectroscopy reveal that amorphous hydrogen phosphate (HPO 4 2- ) modification promotes the adsorption of key intermediates (*CO 3 2- and *COOH), facilitates efficient proton transfer through the establishment of an ordered hydrogen-bonding network (consistent with the Grotthuss mechanism), and stabilizes Zn active sites by acting as a buffer to regulate the local pH environment. These effects collectively enhance the stability and catalytic performance of the catalyst during CO 2 RR. Graphical Bifunctional amorphous phosphate layer simultaneously enhances proton transfer and stabilizes Zn active sites for efficient CO 2 RR. An engineered Zn-HPO 4 overlayer enhances *COOH/*CO 3 2- stabilization and water dissociation while suppressing parasitic hydrogen evolution reactions and Zn dissolution. This synergistic microenvironment regulation delivers 86.4% CO Faradaic efficiency with robust 20 h stability, markedly outperforming pristine Zn catalysts.
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Juhee Jang,Ernest Pahuyo Delmo,Yushen Liu,Guimei Liu,Yinuo Wang,Tiehuai Li,Minhua Shao
Cu-MOFs have shown great potential as electrocatalysts for selective methane production through the carbon dioxide reduction reaction (CO 2 RR). However, achieving coordination-induced tuning over the desired coordination environment of multi-functional Cu-MOFs remains a challenge, which is closely related to regulating the surface binding energy with reactants. Here we develop a modulator-assisted synthesis method for fabricating nanosized Cu-aminoterephthalic acid (Cu-NH 2 BDC) MOFs, aiming to modify the coordination geometry, which leads to the regulation of charge transfer ability. By incorporating a trace amount of 2-methylimidazole (MIm), the crystallinity of Cu-NH 2 BDC can be improved compared to traditional synthesis, which can be attributed to the influence of the coordination environment within the MOFs. The modulation of electrochemical properties, including the redox potential for the evolution of Cu active species and charge transfer resistance, resulting from additional Cu oxidation state by the amino functional groups, contributed to the enhancement of CH 4 FE (63%) and partial current density (−53 mA cm −2 ) in an H-type cell, while effectively suppressing the parasitic hydrogen evolution reaction. This modulator-assisted synthesis approach presents a promising strategy for optimizing the performance of Cu-NH 2 BDC electrocatalysts in CO 2 -to-CH 4 conversion, offering valuable insights into structural modifications and charge transfer processes involved in the reaction.
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DOI
高影响因子
ENERGY & FUELS
·
2026
·
IF 6
Tianxiang Guo,Baijiang Liu,Gujie Yao,Xiaoqing Wang,Yanyan Feng,Da Jin,Xilai Wang,Yarong Du
The electrochemical reduction of CO2 to high-value C2 products, especially ethanol, presents a feasible approach for alleviating greenhouse gas emissions and tackling climate-related challenges. Nevertheless, the rational design of efficient electrocatalysts is still restricted by insufficient activity, suboptimal selectivity, and a limited understanding of the underlying mechanisms. In this study, a hierarchically structured Cu-CoPc/CNT catalyst was fabricated by electrochemical deposition and drop-casting techniques. Comprehensive characterization (BET/SEM/XRD/EDS/XPS) confirmed its electronic configuration and surface properties. Electrochemical evaluations (CV/LSV/EIS/GC/1H NMR) demonstrated an ethanol Faradaic efficiency of 42.3% at a partial current density of 10.65 mA·cm–2, with exceptional ethanol selectivity of 98.6% among C2 products at −1.15 V vs RHE. In conjunction with density functional theory (DFT) calculations, mechanistic investigations have demonstrated that an adequate supply of those intermediates such *COOH and the facilitation of the C–C coupling are the primary factors contributing to the performance improvement of the CO2RR toward ethanol through the synergistic effect between CoPc/CNT and Cu. This research proposes a novel strategy for designing efficient and stable CO2-to-ethanol catalysts, thereby deepening the fundamental understanding of the ethanol formation mechanisms.
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高影响因子
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