VACUUM
·
2024
·
IF 3.8
Xiu Wen,Zhixiu Yang,Lijing Gao,Ruiping Wei,Xiaomei Pan,Jin Zhang,Guomin Xiao
Electrocatalytic reduction of CO 2 affords a potential way to mitigate the greenhouse effect and fuel crisis. In this work, we compared highly-dispersed CuO nanocomposites and Cu–Cu 2 O nanocomposites which all derived from Cu x Al-LDH for CO 2 electrochemical reduction . The Cu–Cu 2 O based nanocomposites obtained through the restoration strategies still retain its layered structure, simultaneously increasing dual Cu–Cu 2 O active sites, which exhibit excellent performance in selective reduction of CO 2 to C 2 H 4 . The Cu 5 Al-ER obtained through in-situ electrochemical reduction is modified by bulk phase, which can regulate active species, increase surface active sites, enhance C–C coupling. Meanwhile, the electrochemical strategy offers numerous benefits, including gentle conditions, adjustable monitoring, exceptional efficiency and adaptability. We have confirmed that cost-effective Cu–Cu 2 O based nanocomposite derived from Cu 5 Al-LDH can effectively promote C–C coupling during electrochemical CO 2 conversion and improve FE C2H4 . The FE C2H4 of Cu 5 Al-ER reaches 36% at −1.2 V vs. RHE. And the current density reaches −172 mA·cm −2 at −1.6 V vs. RHE. The results showed that compared to Cu 5 Al-LDO, the FE C2H4 of Cu 5 Al-ER increased by 2.6 times. In addition, Cu 5 Al-ER exhibits excellent stability during the 12 hours CO 2 catalytic reduction process.
研究领域:
化学
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环境科学
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能源科学
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产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Xu Guangyuan,Peng Xingjie,Wu Chuanqiang,Xi Shibo,Xiang Huixin,Feng Lei,Liu Zhendong,Duan Yi,Gan Lijin,Chen Si,Kong Yuan,Ma Yanzhe,Nie Fujing,Zhao Jie,Hai Xiao,Wei Wei,Zhou Meng,Wang Tianfu,Yao Chuanhao,Zhou Wu,Yan Huan
CO 2 electroreduction to CO promises to give an efficient strategy for CO 2 fixation and transformation. However, current reported active sites fail to deliver sufficient activity with high CO Faradic efficiency (FEco) over a wide range of potential. Here, we show a general synthetic protocol to fabricate a batch of highly pure and active NiN 2 catalysts with precise engineering of the uniform-large ( UL ) vacancy around the active sites, which is accomplished through the ‘pre-deposition + pyrolysis’ of various atomically precise Ni clusters (Ni n ) and in-situ etching of the support by the ‘nano bomb’ (sulfur-ligand in the clusters). The NiN 2 sites with UL vacancies could achieve a high turnover frequency (TOF) of 350000 h −1 with ~100% FEco in a wide potential range of 1500 mV. In-situ infrared spectra and theoretical calculations reveal that a highly pure NiN 2 site with UL vacancy contributes to this remarkable catalytic performance compared to the counterparts. This general synthetic strategy enables us to simultaneously engineer active sites and surrounding vacancies with the employment of atomically precise metal clusters, thereby enhancing catalytic performance for other specific reactions.
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
PubMed
高影响因子
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
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Mengchen Wu,Yang Yang,Jing Zhao,Rui Liu
In CO 2 electroreduction, mutative intermediates and the challenging C C coupling necessitate the spatial interplay between active sites and through dynamically optimizing configurations. Herein, we anchor ethylenediaminetetraacetic acid (EDTA)-bonded Cu x+ /Bi 3+ pair within UiO-66 for a spontaneous spatial-optimizing CO 2 -to-C 2 H 4 electroreduction. Ab initio molecular dynamic (AIMD) simulation visualizes that such metal pair adaptively interacts with intermediates. Density functional theory (DFT) elicits the componential synergy, in which an upshift d-band of Cu activates CO 2 being protonated into *COOH while Bi site stabilizes oxygenated dimers for deep hydrogenation. The dynamic feature of such pair affords large freedom for sorption and migration of various intermediates, which consequently bestows UiO-66-EDTA/CuBi a maximal FE C 2 H 4 of 47 % and a total current density over 100 mA cm −2 in the flow cell.
研究领域:
材料科学
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催化化学
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能源转化
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Progress in Natural Science-Materials International
·
2024
·
IF 4.8
Shijia Liu,Haibin Wang,Xi Wang,Jieshu Zhou,Hongyan Liang
Electroreduction of CO 2 for formic acid production has been regarded as an efficient option for CO 2 utilization. However, under high current, achieving high selectivity for formic acid is challenging, which cannot meet industrial demands. Herein, we reported a type of Bi/In(OH) 3 (BIO) heterojunction reconstructed from Bi 2 S 3 /In(OH) 3 during electrochemical process, in which In(OH) 3 was applied to modulate the electronic structure of Bi. This strategy efficiently enhanced the ∗OCHO intermediates adsorption and lead to a decent selectivity towards formic acid under high current density. BIO displays faraday efficiency of formic acid beyond 95 % across a wide range current density of 200–400 mA cm −2 , where the highest value reached 97.7 % at 400 mA cm −2 . This work clarified the mechanism of CO 2 electroreduction to HCOOH on heterojunction, guiding the design of advanced catalysts.
研究领域:
材料科学
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电化学
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催化反应
✓ 已验证
产品关联
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
✓ 已验证
产品关联
DOI
高影响因子
Chemistry-An Asian Journal
·
2024
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IF 3.5
Yicheng Wang,Qiyu Zhang,Chenxu Wang,Ayeza,Yating Zhang,Chao Hu
The utilization of renewable energy for electrocatalytic carbon dioxide reduction reaction (CO 2 RR) represents a pivotal technology in sustainable carbon conversion. Single-atom catalysts (SACs) featuring transition metal-nitrogen-carbon (M−N−C) structures have demonstrated exceptional electrocatalytic efficacy in CO 2 RR by maximizing atom efficiency. Nevertheless, further investigation is warranted to optimize the catalytic performance of SACs through the selection of suitable carbon sources and supports, as well as the modulation of the microenvironment surrounding individual metal atoms. In this study, a sulfur-doped Ni−N−C catalyst was prepared using a two-step strategy involving metal ion adsorption and thermal decomposition, with porous ion exchange resin serving as the carbon source. Due to the uniform distribution of single atom active centers on the resin-based carbon support and sulfur doping, this catalyst efficiently converts CO 2 into CO with a Faradaic efficiency exceeding 90 % within the range of −0.69~−1.29 V (vs. RHE), reaching a maximum value of 97.7 % (−0.79 V vs. RHE). Theoretical calculations indicate that second-shell sulfur doping effectively promotes coupled transfer of protons and electrons, leading to a significant reduction in Gibbs free energy barriers for CO 2 RR intermediate products.
研究领域:
材料科学
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电化学
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催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 42
·23817-23827
·
IF 12.732
Manman Feng,Xuemei Wu,Huiyuan Cheng,Zihao Fan,Xiangcun Li,Fujun Cui,Shuai Fan,Yan Dai,Guangping Lei,Gaohong He
The diatomic catalysts (DACs) provide a new strategy for efficient catalysis of CO2 reduction reaction (CO2RR) owing to their maximum atomic utility and more flexible active sites. However, it is still challenging to precisely design heteronuclear diatomic active centers and understand the coordination mechanism of binary sites at the atomic level. Herein, a nitrogen-doped carbon matrix with precisely controlled Fe–Cu diatom sites is synthesized through a metal–organic framework. The as-obtained Fe/Cu–N–C catalyst exhibits an excellent CO faradaic efficiency (>95% over a wide potential range of −0.4 to −1.1 V vs. RHE, 99.2% at −0.8 V vs. RHE), a high turnover frequency (5047 h−1 at −1.1 V vs. RHE), and a low overpotential (50 mV), thus outperforming most reported atomically dispersed catalysts. Further density functional theory calculations indicate that the synergy between Fe–Cu diatoms causes rapid charge transfer and effectively adjusts the position of the d-band center, which reduces the energy barriers for *COOH formation and *CO desorption. This work provides a new approach for advancing universal synthesis strategies to construct heteronuclear diatomic catalysts and explore synergistic effects.
研究领域:
材料科学
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催化化学
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能源转换
✓ 已验证
DOI
高影响因子
Small
·
2025
·
IF 12.1
Haixin Sun,Xupeng Qin,Yuhao Zhang,Yanzhi Xu,Yaling Jiang,Fengwen Pan,Qinghua Liu
Coordination reconstruction of atomically dispersed active sites in electrocatalytic reactions is expected to enhance the catalytic activity, but achieving this goal remains challenging. Herein, a single-atom‒nanoparticle synergistic catalyst composed of pyridine Fe─N sites and Ni nanoparticles (NPs) encapsulated in nitrogen-doped carbon nanotubes is presented, in which the Ni NPs can reconstruct the Fe─N─C coordination structure from Fe─N 4 to Fe─N 2 through the carbon nanotube structure during the CO 2 electroreduction reaction. The catalyst exhibites a low onset potential of −0.12 V in an alkaline flow cell, with a high Faradaic efficiency for CO (FE CO ) greater than 97% over a wide potential range of −0.4–−1.2 V and a maximum FE CO of 98.7%. In situ X-ray absorption spectroscopy and infrared characterization results demonstrate that the reduction in the Fe─N coordination number during the reaction process promotes the protonation of CO 2 to form the * COOH intermediate and thereby significantly improves the CO 2 electroreduction performance.
研究领域:
材料科学
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电催化
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
·
2025
·
IF 16.9
Wuyi Zhang,Asad Mehmood,Ghulam Ali,Hui Liu,Liyuan Chai,Jun Wu,Min Liu
Unsaturated Ni single atom catalysts (SACs), Ni-Nx (x=1,2,3), have been investigated to break the conventional Ni-N4 structural limitation and provide more unoccupied 3d orbitals for CO2RR intermediates adsorption, but their intrinsically low structural stability has seriously hindered their applications. Here, we developed a strategy by integrating Ni nanoclusters to stabilize unsaturated Ni-N3 atomic sites for efficient CO2 electroreduction to CO at industrial-level current. DFT calculations revealed that the incorporation of Ni nanocluster effectively stabilizes the unsaturated Ni-N3 atomic sites and modulates their electronic structure to enhance the adsorption of the key intermediate *COOH during CO2RR. Guided by these insights, we prepared an optimal composite catalyst, Ni6@Ni-N3, which features a Ni6N6 nanocluster surrounded by six Ni-N3 single atoms sites, through low-temperature pyrolysis. As a result, Ni6@Ni-N3 demonstrated a remarkably high CO Faradaic efficiency (FECO) of 99.7% and a turnover frequency (TOF) of 83984.2 h-1 at 500 mA cm-2 under -1.15 VRHE, much better than the conventional Ni-N4 . XAS analyses of Ni6@Ni-N3 before and after long-term CO2RR testing confirmed the excellent stability of its coordinative environment. This work highlights a generalizable approach for stabilizing unsaturated single-atom catalysts, paving the way for their application in high-performance CO2RR.
研究领域:
材料科学
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催化化学
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能源转换
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Huan Wang,Shu-Wei Yin,Jianchuan Liu,Weitao Wang,Zhen-Hong He,Kuan Wang,Zhi-Hao Zhao,Zhao-Tie Liu
Ni, especially Ni single atom catalysts (SACs) are the most promising electrocatalyst in the reduction of CO 2 to CO. However, the high energy barrier for the formation of *COOH on Ni SA sites leads to a high overpotential for CO 2 RR, which severely hinders the CO production efficiency. How the coupling effect of Ni SAs and Ni nanoparticles (NPs) sites improve the performance of Ni-based electrocatalysts is interesting to be investigated. Herein, theoretical calculations revealed that the synergy of Ni SAs and Ni NPs could efficiently lower the energy barrier of the *COOH formation via promoting the H 2 O dissociation process to accelerate the *H supply for CO 2 protonation as well as promote the CO 2 adsorption and CO desorption, thus improving catalytic activity. Based on the theoretical study, Ni-N 4 SA coupled with Ni nanoparticles supported on nitrogen-doped carbon nanotubes (Ni-N 4 Ni NP /NCNT) was designed. As electrocatalyst, the Ni-N 4 Ni NP /NCNT showed an ultralow onset overpotential of 60 mV for CO 2 RR-to-CO, and achieves a FE CO of ∼99 % from an overpotential of as low as 160 mV, outperforming state-of-the-art Ni SACs. This work not only sheds new light for the rational synthesis of Ni-based catalysts with both Ni SAs and Ni NPs sites to achieve efficient CO 2 RR to CO, but also offers an in-depth insight for the origin of efficient performance of cooperative Ni SA -Ni NP catalysts.
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Jianhua Shen,Zhenping Pan
Dual-atoms catalysts (DACs), while inheriting the advantages of maximum atom utilization ratio and excellent selectivity of single-atom catalysts (SACs), can better enhance the catalytic activity through the synergy of adjacent atoms. Therefore, DACs are considered to be very potential catalysts for CO 2 to CO conversion. Its catalytic activity is greatly influenced by the coordination environment and morphology. Here, hollow urchin-like Ni N C catalysts (Ni-NC(HU)-x, x = 100, 50, 25, 0) were synthesized using urchin-like nickel particles as template. By adjusting the amount of additional nitrogen source, the percentage content of pyridinic-N was adjusted as well as further affecting the coordination environment. Among them, Ni-NC(HU)-50, which had the highest content of pyridinic-N, formed a dual-atoms coordination structure and had the best catalytic performance that the CO Faradaic efficiency (FE CO ) reached 97.2 % at −0.9 V vs. reversible hydrogen electrode (RHE) and sustained above 95 % within 50 h. In-situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and density functional theory (DFT) calculations showed that Ni-NC(HU)-50 exhibited the best performance of CO 2 reduction reaction (CO 2 RR) by lowering the *COOH formation free energy barrier and its favorable dual desorption mechanism of *CO L and *CO B .
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）