ELECTROCHIMICA ACTA
·
2023
·
IF 6.6
Zhihong Xu,Yunxi Han,Jiuyi Sun,Meng Xu,Wenli Zhao,Qingfa Wang
Electrochemical CO 2 reduction (ECR) to C 2+ products is an efficient method to accomplish intermittent energy storage and CO 2 utilization. Developing high-selectivity electrocatalysts for C 2+ products, especially C 2+ alcohols, have attracted more attention but still remains a major challenge. Here, three kinds of short nanotube (<100 nm), long nanotube (>100 nm), and long nanotube-assembled hollow sphere CuSiO 3 catalysts with different confined space are fabricated for boosting the ECR to produce C 2+ products selectivity. Long CuSiO 3 nanotubes exhibit a higher yield of C 2+ alcohols (26.8 %) and more satisfactory Faraday efficiency (FE) of 69.5 % for C 2+ products than short nanotubes and nanotube-assembled hollow spheres. The confinement effect of long CuSiO 3 nanotubes is conducive to promoting the dimerization of the key reaction intermediate (*CO), inhibiting the diffusion of protons and the side-reaction hydrogen evolution reaction (HER). The formed Cu 0 /Cu + interfaces in CuSiO 3 nanotubes promote the dimerization reactions of adsorbed *CO. The synergistic effect of nanotubes confinement and Cu 0 /Cu + interfaces facilitate the C C coupling reaction to C 2+ products via ECR.
研究领域:
材料科学
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电化学
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能量存储与转换
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产品关联
DOI
高影响因子
Catalysts
·
2021
·Vol. 11
·期 5
·535
·
IF 4.146
Shuaikang Zhu,Xiaona Ren,Xiaoxue Li,Xiaopo Niu,Miao Wang,Shuang Xu,Zheyuan Wang,Yunxi Han,Qingfa Wang
The copper-based catalyst is considered to be the only catalyst for electrochemical carbon dioxide reduction to produce a variety of hydrocarbons, but its low selectivity and low current density to C2products restrict its development. Herein, a core-shell xZnO@yCu2O catalysts for electrochemical CO2reduction was fabricated via a two-step route. The high selectivity of C2products of 49.8% on ZnO@4Cu2O (ethylene 33.5%, ethanol 16.3%) with an excellent total current density of 140.1 mA cm−2was achieved over this core-shell structure catalyst in a flow cell, in which the C2selectivity was twice that of Cu2O. The high electrochemical activity for ECR to C2products was attributed to the synergetic effects of the ZnO core and Cu2O shell, which not only enhanced the selectivity of the coordinating electron, improved the HER overpotential, and fastened the electron transfer, but also promoted the multielectron involved kinetics for ethylene and ethanol production. This work provides some new insights into the design of highly efficient Cu-based electrocatalysts for enhancing the selectivity of electrochemical CO2reduction to produce high-value C2products.Keywords:CO2electrochemical reduction;core-shell structure;ZnO@Cu2O;synergy effect;C2products selectivity
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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环境科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Taotao Zhao,Chenyang Shen,Gui Liu,Jun Yao,Xianghao Wang,Huajie Tao,Yu He,Yuchi Liu,Zhewei Zhang,Feifei Mei,Xiangke Guo,Luming Peng,Yan Zhu,Xuefeng Guo,Nianhua Xue,Weiping Ding
We report here a high-performance catalyst ReMoS x @HSSZ-39 compounded with SAPO-34 for conversion of CO 2 to C 2-4 hydrocarbons, in which the ReMoS x clusters are responsible for highly efficient hydrogenation of CO 2 to methanol as the intermediate and then the surrounding zeolitic acid sites for further conversion of methanol to hydrocarbons. The investigation finds that uniform ReMoS x clusters can be reliably fabricated in zeolitic cages by co-introduction of rhenium and molybdenum species into the HSSZ-39 zeolite and followed by sulfidation, which constitutes an intimate bifunction catalyst through better cooperation of ReMoS x clusters and the zeolitic acid sites. Compared with MoS x @HSSZ-39, the introduction of rhenium significantly suppresses CO generation. By mixing some SAPO-34 zeolite, with increased density of protonic acid, more than 86 % C 2-4 hydrocarbons in organic products and only 21 % CO at 32.5 % of CO 2 conversion are obtained and the composite catalyst shows excellent stability with more than 95 % C 2-4 hydrocarbons in organic products, less than 30 % CO and above 26.6 % of CO 2 conversion after 1000 h on stream.
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
JOURNAL OF POWER SOURCES
·
2014
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IF 5.211
Bencai Lin,Fuqiang Chu,Yurong Ren,Baoping Jia,Ningyi Yuan,Hui Shang,Tianying Feng,Yuanyuan Zhu,Jianning Ding
Novel C2-substituted imidazolium-based cross-linked anion exchange membranes (AEMs) are prepared via irradiation with ultraviolet light cross-linking of styrene, acrylonitrile and 1,3-diallyl-2-methyl imidazolium bromine ([DAMIm][Br]), and followed by anion exchange with hydroxide ions. [DAMIm][Br] is synthesized and used both as crosslinker and hydrophilic phase. The ionic conductivity of the AEMs increases with increasing [DAMIm][Br] content due to the hydrophilic regions and the continuous hydrophilic polymeric networks formed in the membranes. The imidazolium-based cross-linked AEMs show excellent thermal stabilities, and the membrane which containing 30% mass fraction of [DAMIm][Br] shows ionic conductivity up to 2.0 × 10 −2 S cm −1 and good long-term chemical stability in 1 M KOH solution. The results of this study suggest that the C2-substituted imidazolium-based cross-linked AEMs have good perspectives for alkaline fuel cell applications .
研究领域:
材料科学
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能源工程
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DOI
高影响因子
JOURNAL OF APPLIED TOXICOLOGY
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2019
·Vol. 39
·期 12
·1640-1650
·
IF 3.065
Yicong Chang,Feng Wang,Yang Yang,Yuanyuan Zhang,Ishfaq Muhammad,Rui Li,Changwen Li,Ying Li,Chenxi Shi,Xin Ma,Beili Hao,Fangping Liu
Acetaminophen (APAP) is an antipyretic and analgesic, which is commonly associated with drug-induced hepatic injury. C2-ceramide plays a key role in mediating cell life activities, and oltipraz was extensively studied as a cancer chemopreventive agent. Glutathione S -transferase A1 (GSTA1) acts as a vital liver detoxification enzyme. Hepatocyte nuclear factor 1 (HNF-1) regulates various cellular signaling pathways. In this study, we investigated the effects of C2-ceramide and oltipraz on APAP-induced hepatocyte injury and the changes of HNF-1 and GSTA1. Results showed that C2-ceramide (6 μmol/L) exacerbated APAP-induced hepatocyte injury and caused a significant decrease ( P < .01) in HNF-1 and GSTA1 expressions. Meanwhile, GSTA1 content in supernatant was significantly increased ( P < .01). In contrast, oltipraz (8 μmol/L) reduced the injury and significantly elevated ( P < .01) HNF-1 and GSTA1 expressions while GSTA1 content in supernatant was significantly decreased ( P < .01). In conclusion, these findings revealed that C2-ceramide inhibited HNF-1 and GSTA1 expression and exacerbated hepatocyte injury, while oltipraz treatment results in the reduction of hepatocyte injury, and promoted HNF-1 and GSTA1 expression. Additionally, the changes in HNF-1 and GSTA1 were related to APAP-induced hepatocyte injury. These results were useful to investigate the mechanism of an antipyretic and analgesic drug combination.
研究领域:
药理学
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毒理学
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分子生物学
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产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2023
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IF 9.5
Jilin Liu,Kai Yu,Qianlong Zhu,Zhiyuan Qiao,Hong Zhang,Jie Jiang
Electroreduction of carbon dioxide (CO2) to C2 products (ethylene and ethanol) using efficient catalysts is a feasible approach to alleviate the climate crisis. Cuprous oxide nanoparticles (Cu2O NPs) are a promising catalyst for C2 production but suffer from inherent selectivity and durability. To address this challenge, a Cu2O NPs-nitrogen-doped carbon nanotube (Cu2O NPs-NCNT) composite was prepared with carbon nanotubes (CNTs), Cu2O NPs, and phthalocyanine (Pc). The results indicate that Cu2O NPs-NCNT has excellent Faradic efficiency of C2 products (77.61%) at −1.1 V vs RHE, which is 103.43% higher than that of Cu2O NPs. In the potentiostatic electrolysis combined with Raman spectroscopy and X-ray photoelectron spectroscopy (XPS) measurements, Cu2O NPs-NCNT exhibited structural and catalytic current stability over 10 h. Finally, density functional theory calculations combined with XPS demonstrated that the NCNT in Cu2O NPs-NCNT can selectively absorb CO2 through specific N–CO2 interactions. Our work provides a unique strategy to promote the selectivity of Cu2O NPs for C2 production by introducing N-doped linear carbon materials to fabricate composite.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2025
·
IF 4.7
Minggang Hu,Xiaochen Wang,Can Wang,Hongtao Chu,Xinfeng Song,Guohua Dong,Jiyuan Zhang,Jin Xing
In this study, a new and simple method for synthesizing boron complexes was presented. The boron complexes with C 2 -symmetric ligands were prepared from in situ generated tertiary amine by the reaction of salicylaldehyde with primary amine in the presence of sodium borohydride. The boron complexes were characterized by 1 H and 13 C NMR spectroscopy, elemental analysis, and mass spectrometry. The crystal structures of complexes 1 and 2 were determined by single crystal X-ray diffraction method. The complex is a mononuclear boron complex with a tertiary amine ligand. The boron center is tetracoordinated with a distorted tetrahedral geometry. Catalytic activities of the boron complexes in the reduction of dyes, was investigated using sodium borohydride as a reducing agent. Complexes 1 and 2 were effective catalysts for degradation of dyes. Kinetic studies reveal that the reduction of methylene blue is of the first order. Free radical scavenging activities of the boron complexes have been tested using DPPH, ABTS and hydroxyl radicals, respectively. The result shows that the boron complexes have effective antioxidant activity.
研究领域:
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
Journal of Physical Chemistry C
·
2023
·
IF 3.7
Yuanjiao Liu,Yi Wang,Songyao Zhang,Hengqi Zou,Xinrui Miao,Wenli Deng
The self-assembly of two kinds of C2-symmetric aromatic carboxylic acids named 4,4′,4″,4‴-(1,4-phenylenebis(azanetriyl))tetrabenzoic acid (H4PTA) and 5′,5″-bis(4-carboxyphenyl)-[1,1′:3′,1″:3″,1‴-quaterphenyl]-4,4‴-dicarboxylic acid (H4QDA) and the coadsorption with coronene (COR) molecules at different solution concentrations were investigated at the heptanoic acid (HA)/highly oriented pyrolytic graphite (HOPG) interface by scanning tunneling microscopy (STM). H4PTA molecules with nonplanar conformation self-assembled into a highly ordered rhombus structure at variational concentrations and subsequently could be regulated into a Kagomé network by the coadsorption of COR molecules. H4QDA molecules with planar conformation self-assembled into two various nanostructures (rhombus structure and Kagomé network) coexisting on the HOPG surface at different concentrations. The Kagomé architecture of H4QDA could act as a rigid host template to trap the COR molecules. Meanwhile, COR exhibited preferential adsorption in the porous template: COR only entered the hexagonal cavities at low concentrations and filled in all hexagonal and triangular cavities at high concentrations. Density functional theory (DFT) calculations and molecular dynamics (MD) simulations showed that the host–guest co-assembled structures were more thermodynamically and kinetically stable. The formation of different self-assembly and co-assembly processes of two molecules could be attributed to the dissimilar molecular conformation. Our work is of significance to further explore the formation mechanism of two-dimensional (2D) porous arrangements and provides an ideal way to regulate the adsorption of porous templates.
研究领域:
材料科学
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表面科学
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计算化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Canyan Yang,Ruichen Wang,Chao Yu,Jinhua Xiao,Zhiwei Huang,Bihong Lv,Huawang Zhao,Xiaomin Wu,Guohua Jing
Cu-based catalysts inevitably undergo surface reconstruction during the electrochemical carbon dioxide reduction reaction (CO 2 RR) process. Thus, it is a challenge to construct stable Cu + -Cu 0 sites of Cu-based catalysts. In this study, we report a simple and facile engineering strategy for stable Cu + -Cu 0 sites and oxygen defects derived from the boron-doped copper composite catalyst (B-Cu x O) as an efficient CO 2 RR electrocatalyst. The 5 % B-Cu x O exhibited 48.44 % C 2+ products Faraday efficiency (FE) for 12 h at −1.0 V vs reversible hydrogen electrode (RHE) in H-cell, which was far superior to Cu x O (23.85 %). Combining density functional theory (DFT) and in situ Attenuated Total Reflection Fourier Transform Infrared spectroscopy ( in situ ATR-FTIR), a higher electronic depletion on the catalyst surface inhibited the electrons accumulation around Cu sites, thereby maintaining the positive charge and inhibiting the complete reduction of Cu + . Moreover, the high oxygen defects in 5 % B-Cu x O could effectively activate CO 2 into *CO. We emphasized that Cu + functioned as the primary active site by facilitating adsorption and dimerization of *CO, whereas Cu 0 assisted in optimizing CO 2 activation.
研究领域:
材料科学
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电化学
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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
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催化反应
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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
Ren Bohua,Zhang Xiaowen,Yang Leixin,Wen Guobin,Dong Silong,Xiong Haoyang,Liu Yiyin,Duan Xiaoman,Tan Lichao,Wang Xin,Chen Zhongwei
Electrocatalytic upgrade of CO 2 offers a promising approach for recycling of global CO 2 emissions, facilitating the achievement of carbon neutrality. Nevertheless, direct utilization of practical dilute CO 2 is urgently important yet rather difficult, which is hindered by the balance of reaction kinetics and mass transport of CO 2 to the catalytic sites. Herein, we propose coordinating the local environment and active catalyst by constructing covalent organic frameworks (COF) on single-atomic In-doped Cu 2 O (In 1 @Cu 2 O) for a high tolerance of CO 2 inlet concentrations (15% to 100%). The optimized amounts of COF functionalized by the trifluoromethyl group act as the local CO 2 /CO diffusion channels via steric confinement effects and C···F electronic effects. Besides, the formation of key intermediates for C 2+ products is greatly facilitated by the promoted COOH adsorption. Hence, a total current of 81.7 A is realized in a 4 × 100 cm 2 electrolyzer stack with over 770 mmol/h C 2+ products at an inlet of dilute CO 2 . Such a electrode architecture sheds light on the dilute CO 2 electrolysis at the potential industrial scale.
研究领域:
电化学
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环境催化
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能源材料
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碳中和
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工业电解
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science Advances
·
2023
·Vol. 9
·期 24
·
IF 13.6
Mingrui Wang,Peng Wang,Guanghui Zhang,Zening Cheng,Mengmeng Zhang,Yulong Liu,Rongtan Li,Jie Zhu,Jianyang Wang,Kai Bian,Yi Liu,Fanshu Ding,Thomas P. Senftle,Xiaowa Nie,Qiang Fu,Chunshan Song,Xinwen Guo
The decomposition of cobalt carbide (Co 2 C) to metallic cobalt in CO 2 hydrogenation results in a notable drop in the selectivity of valued C 2+ products, and the stabilization of Co 2 C remains a grand challenge. Here, we report an in situ synthesized K-Co 2 C catalyst, and the selectivity of C 2+ hydrocarbons in CO 2 hydrogenation achieves 67.3% at 300°C, 3.0 MPa. Experimental and theoretical results elucidate that CoO transforms to Co 2 C in the reaction, while the stabilization of Co 2 C is dependent on the reaction atmosphere and the K promoter. During the carburization, the K promoter and H 2 O jointly assist in the formation of surface C * species via the carboxylate intermediate, while the adsorption of C * on CoO is enhanced by the K promoter. The lifetime of the K-Co 2 C is further prolonged from 35 hours to over 200 hours by co-feeding H 2 O. This work provides a fundamental understanding toward the role of H 2 O in Co 2 C chemistry, as well as the potential of extending its application in other reactions.
研究领域:
催化化学
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化学工程
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材料科学
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可持续能源
·
多相催化
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DOI
高影响因子
危险品化学品经营许可证（带存储）