Journal of Environmental Sciences
·
2025
·
IF 6.3
Canyan Yang,Wei Liu,Zhao Zuo,Jinhua Xiao,Huawang Zhao,Bihong Lv,Zuoming Zhou,Xiaomin Wu,Guohua Jing
Carbon-carbon (C-C) coupling, the rate-determining step in electrocatalytic CO 2 reduction reaction (CO 2 RR) to C 2+ products, has low efficiency and poor stability. It originates from an ineffective water dissociation capability and a high energy barrier for the C-C coupling pathway on existing catalysts. Herein, an efficient and facile Br-CuO electrocatalyst was synthesized to promote water dissociation and achieve an impressive Faradic Efficiency (FE) of around 60% C 2 H 4 at a current density of up to -350 mA/cm 2 with stability of 16 h. Combinative theoretical and experimental protocols strongly evidence that the architecture of Cu 0 -Cu + sites is crucial for the enhancement in CO 2 RR activity. Cu 0 activates CO 2 and Cu + strengthens *CO adsorption to further boost C-C coupling. Furthermore, Br doping can facilitate the dissociation of water to generate *H, which promotes the protonation of *CO to *CHO, thereby enabling the low energy barrier asymmetric *CHO-*CO coupling. The in situ ATR-FTIR and Density functional theory (DFT) was analyzed to explain the reaction mechanism and pathway. This study elucidates the critical function of water dissociation and provides a promising avenue to efficient CO 2 -to-C 2 H 4 electrocatalysis.
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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能量转换
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环境科学
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DOI
高影响因子
Polymers
·
2026
·Vol. 18
·期 11
·1398
·
IF 5.8
Jianing Zong,Kaize Si,Jingjing Li,Xiaomei Wang,Xu Zhang
SiOxanodes are highly promising for next-generation lithium-ion batteries due to their superior theoretical capacity. However, issues such as drastic volume expansion and low initial Coulombic efficiency (ICE) impede their practical use. While macroporous architectures can mitigate these challenges, traditional fabrication often depends on tedious hard templating methods and significant organic solvent consumption. In this work, we report a sustainable, emulsion-self-templated and organic solvent-free strategy to synthesize a carbon-coated 3D macroporous SiOx/C composite (3DM-SiOx/C@C). Our approach uniquely integrates radical polymerization with a water-in-oil emulsion and sol–gel process, followed by chemical vapor deposition (CVD). The 3D macroporous framework is generated via in-situ emulsion droplets acting as self-templates, effectively eliminating the need for external sacrificial templates and toxic etchants. Notably, this organic solvent-free process achieves an exceptional precursor to (precursor + organic solvent) mass ratio of 1.0, contrasting sharply with conventional methods (0.0044–0.17). The resulting hierarchical structure, characterized by interconnected macropores and a uniform carbon coating, significantly enhances structural integrity and electronic conductivity. Electrochemical evaluations reveal that 3DM-SiOx/C@C exhibits an improved ICE of 74.32% and long-term cycling stability even at a high current density of 1.0 A g−1compared to non-porous and uncoated counterparts. This integrated synthesis offers a green and scalable pathway for developing high-performance silicon-based anodes for large-scale energy storage.
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PubMed
高影响因子
Small
·
2023
·Vol. 20
·期 3
·2304990
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IF 13.3
Na Ye,Wenchao Sheng,Riguang Zhang,Binhang Yan,Zhao Jiang,Tao Fang
The splitting of the C–C bonds of ethanol remains a key issue to be addressed, despite tremendous efforts made over the past several decades. This study highlights the enhancement mechanism of inexpensive NbN-modified Pd 1 Sn 3 -NbN/C towards the C–C bonds cleavage for alkaline ethanol oxidation reaction (EOR). The optimal Pd 1 Sn 3 -NbN/C delivers a catalytic activity up to 43.5 times higher than that of commercial Pd/C and high carbonate selectivity (20.5%) toward alkaline EOR. Most impressively, the Pd 1 Sn 3 -NbN/C presents good durability even after 25 200 s of chronoamperometric testing. The enhanced catalytic performance is mainly due to the interfacial interaction between PdSn and NbN, demonstrated by multiple structural characterization results. In addition, in situ ATR-SEIRAS (Attenuated total reflection-surface enhanced infrared absorption spectroscopy) results suggest that NbN facilitates the C–C bonds cleavage towards the alkaline EOR, followed by the enhanced OH adsorption to promote the subsequent oxidation of C1 intermediates after doping Sn. DFT (density functional theory) calculations indicate that the activation barriers of the C–H bond cleavage in CH 3 CH 2 OH, CH 3 CHOH, CH 3 CHO, CH 3 CO, CH 2 CO, and the C–C bond cleavage in CH 3 CO, CH 2 CO, CHCO are evidently reduced and the removal of adsorbed CH 3 CO and CO becomes easier on the PdSn-NbN/C catalyst surface.
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PubMed
高影响因子
MATERIALS & DESIGN
·
2018
·
IF 4.525
Haibo Ouyang,Guibiao Li,Cuiyan Li,Jianfeng Huang,Jie Fei,Jing Lu
C/C-Zr-Si-O composites were prepared by carbothermal reduction of hydrothermal co-deposited ZrO 2 , SiO 2 , and C. The bulk density of composites reached 1.71 g/cm 3 with 8 cycles of co-deposition. The matrix of the composites includes ZrC, SiC, ZrO 2 , and SiO 2 with fine grain size (300–500 nm) and homogeneous distribution. The mass and linear ablation rate of C/C-Zr-Si-O composites were 0.112 mg/cm 2 ·s and 0.46 μm/s, respectively, under a plasma flame for 120 s. The attractive ablation resistance of the composites resulted from its unique structure, which tends to form a continuous ZrO 2 -SiO 2 glass layer in the ablation center, a layer of SiO 2 -ZrO 2 bubbles in the transition region, and fluffy SiO 2 nanowires layer in the heat-affected region. These ablation layers were barriers to restrain the diffusion of oxidative gas and heat. The C/C-Zr-Si-O composites provide an alternative ceramics system with attractive ablation resistance, while carbothermal reduction of hydrothermal co-deposited oxides is a feasible method for the structural design of carbon fiber reinforced ultra-high temperature ceramic.
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高影响因子
ANALYST
·
2022
·Vol. 147
·期 7
·1341-1347
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IF 5.227
Chen-Chen Jiang,Xiao-Chong Li,Jian-Ang Fan,Jia-Ying Fu,Xu-Nan Huang-Fu,Jia-Jie Li,Ju-Fang Zheng,Xiao-Shun Zhou,Ya-Hao Wang
The electroreductive cleavage of carbon–halogen bonds has attracted increasing attention in both electrosynthesis and pollution remediation. Herein, by employing the in situ electrochemical shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) technique, we have successfully investigated the electroreductive dehalogenation process of aryl halides with the thiol group on a smooth Au electrode in aqueous solution at different pH values. The obtained potential-dependent Raman spectra directly reveal a mixture of the reduction products 4,4′-biphenyldithiol (BPDT) and thiophenol (TP). The conversion ratios of the C–Cl and C–Br bonds at pH = 7 are 37% and 55%, respectively. Furthermore, quantitative analysis of the intensity variations of ν(C–Cl), ν(C–Br) and aromatic ν(CC) stretching modes suggests electroreductive dehalogenation via both direct electron transfer reduction and electrocatalytic hydrodehalogenation. Molecular evidence for the C–C cross coupling process through TP reaction with benzene free radical intermediates is found at negative potentials, which leads to the increasing selectivity of biphenyl products.
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PubMed
高影响因子
CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Chen Zeng,Mingyu Zhang,Hanwei He,Xiaodong Wang,Kai Tong,Yafeng Wang,Ping Xu,Lei Zheng,Guang Zeng,Zhean Su,Qizhong Huang
Sol-gel is a promising technology to prepare the C/C–ZrC–SiC composites. However, carbon fiber erosion caused by carbothermal reduction severely degrades properties of the composites. At present study, the addition order of carbon source during sol-gel process was optimized to improve the microstructure, mechanical property and ablation resistance of the composites. Results show that adding phenolic resin before gelation combined with deposited pyrocarbon interlayer around the carbon fibers can greatly alleviate the degradation of the C/C–ZrC–SiC composites by reducing the carbon fiber erosion. The composites thus prepared delivered the flexural strength , mass and linear ablation rates are 162.58 MPa, 0.147 mg/(cm 2 ⋅s) and 0.0098 mm/s, respectively, which are 449% higher, 9.26% lower and 38.36% lower than those of the counterpart that added phenolic resin after gelation. The excellent performance is attributed to little erosion of the carbon fibers and the dense matrix of ZrC–SiC ceramics obtained from adding carbon source before gelation during the sol-gel process.
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高影响因子
RSC Advances
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2015
·Vol. 5
·期 117
·96372-96376
·
IF 3.84
Zheng-Jun Wang,Peng-Hui Wang,Jing-Jing Lv,Jiu-Ju Feng,Xinhua Xu,Ai-Jun Wang,Chak-Tong Au,Renhua Qiu
Commercial copolymer Luviset clear (L1), an environmentally benign and efficient ligand, was used to facilitate the catalytic performance of Cu(NO3)2 for homo-coupling of terminal alkynes. A series of substituted aromatic and aliphatic terminal alkynes were investigated. It was found that Cu(NO3)2@L1 can catalyze the C–C coupling reactions without any other base, and the corresponding diynes are generated in good to excellent yield. X-ray photoelectron spectroscopy was used to study the reaction mechanism, and the results evidence a Cu(II)/Cu(I) catalytic system. Additionally, the catalyst can be easily separated and reused without showing significant loss of catalytic activity.
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高影响因子
CORROSION SCIENCE
·
2015
·
IF 4.422
Dong Huang,Mingyu Zhang,Qizhong Huang,Liping Wang,Liang Xue,Xian Tang,Kejian He
C/C–ZrB 2 –ZrC–SiC composites were fabricated by polymer infiltration and pyrolysis (PIP) with a preform of C f /ZrB 2 . The ZrB 2 powders were sprayed onto fabric layer by layer before the fabric is needled. After introduction of resin carbon and ZrC–SiC into the preform, a ceramic coating on the matrix and fibres was formed in the composites. The plasma ablation test indicates that the composites possess a good ablation resistance after ablation for 180 s and 240 s. The SiO 2 –ZrO 2 barrier layer, high temperature Zr–Si–O glass layer and heat dissipation all contribute to the good ablation resistance of the composites.
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DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·Vol. 34
·期 44
·2405922
·
IF 18.5
Minmin Ma,Ran Wang,Li Shi,Ronghua Li,Jie Huang,Zhuo Li,Peng Li,Elena Yu. Konysheva,Yanbo Li,Gang Liu,Xiaoxiang Xu
Photocatalytic carbon-carbon (C─C) coupling of benzyl alcohol is a promising means to coproduce the value-added chemicals with H 2 but is generally subject to low efficiency in terms of photon utilization. Here, efficient benzyl alcohol C─C coupling is achieved over Zn 2 In 2 S 5 containing a tunable content of Zn vacancies ( V Zn ). The V Zn tends to form shallow defect states below the conduction band that can expedite photocarrier separation by collecting the photo-generated electrons. The V Zn -collected electrons are essential for a high selectivity of the C─C coupling reactions because they enable a fast elimination of the byproduct benzaldehyde by catalyzing its reduction back to the ketyl radicals. Under simulated sunlight, the V Zn -containing Zn 2 In 2 S 5 accomplishes ≈100% conversion of benzyl alcohol for merely 1 h and attains ≈100% selectivity for the C─C coupling compounds for 2 h, delivering an apparent quantum yield as high as 7.7% at 420 ± 20 nm. The benefits of V Zn have also been verified by the theoretical calculations that indicate reduced energy barriers for various surface reactions in the presence of V Zn . This work brings fresh mechanistic insights into the role of V Zn and can serve as a useful guideline in the design of efficient photocatalysts.
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高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Wang Shifu,Li Fuhua,Zhao Jian,Zeng Yaqiong,Li Yifan,Lin Zih-Yi,Lee Tsung-Ju,Liu Shuhui,Ren Xinyi,Wang Weijue,Chen Yusen,Hung Sung-Fu,Lu Ying-Rui,Cui Yi,Yang Xiaofeng,Li Xuning,Huang Yanqiang,Liu Bin
Manipulation C-C coupling pathway is of great importance for selective CO 2 electroreduction but remain challenging. Herein, two model Cu-based catalysts, by modifying Cu nanowires with Ag nanoparticles (AgCu NW) and Ag single atoms (Ag 1 Cu NW), respectively, are rationally designed for exploring the C-C coupling mechanisms in electrochemical CO 2 reduction reaction (CO 2 RR). Compared to AgCu NW, the Ag 1 Cu NW exhibits a more than 10-fold increase of C 2 selectivity in CO 2 reduction to ethanol, with ethanol-to-ethylene ratio increased from 0.41 over AgCu NW to 4.26 over Ag 1 Cu NW. Via a variety of o perando /in-situ techniques and theoretical calculation, the enhanced ethanol selectivity over Ag 1 Cu NW is attributed to the promoted H 2 O dissociation over the atomically dispersed Ag sites, which effectively accelerated *CO hydrogenation to form *CHO intermediate and facilitated asymmetric *CO-*CHO coupling over paired Cu atoms adjacent to single Ag atoms. Results of this work provide deep insight into the C-C coupling pathways towards target C 2+ product and shed light on the rational design of efficient CO 2 RR catalysts with paired active sites.
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DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Tianxiang Guo,Zijun Men,Xiaoqing Wang,Gujie Yao,Baijiang Liu,Xilai Wang,Yarong Du,Da Jin
Electrochemical carbon dioxide reduction reactions (ECO 2 RR) for ethanol synthesis represents a highly valuable yet challenging objective, mainly due to the low selectivity and elusive formation mechanism. This study aims to address this challenge by designing a pulsed-electrodeposited bimetallic CuAg catalyst. The surface morphology and elemental valence state distribution of the CuAg catalyst were comprehensively characterized using BET/SEM/EDS/XRD/XPS techniques. Subsequently, the electrocatalytic performance was systematically investigated based on CV/LSV/EIS/GC/ 1 H NMR methods. The results indicated that the CuAg catalyst attained a Faradaic efficiency of 11.39 % for ethanol production at a current density of 84 mA·cm −2 , along with an ethanol/ethylene selectivity of 8.26. In combination with the analysis of DFT calculations, the incorporation of Ag into the Cu catalyst enhanced the catalytic performance primarily through three mechanisms: increasing the specific surface area and porosity to generate more Cu active sites and high ESCA , modifying the electronic structure of Cu atoms to facilitate the C–C coupling pathway, and reducing the interfacial resistance to promote reaction kinetic rates. These findings provide atomic-level insights into the ECO 2 RR mechanism and establish a novel paradigm for the design of bimetallic catalysts to achieve the efficient synthesis of multi-carbon fuels such as ethanol.
研究领域:
电催化
·
能源化学
·
材料化学
·
表面科学
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环境化学
·
物理化学
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DOI
高影响因子
RARE METALS
·
2024
·Vol. 43
·期 4
·1513-1523
·
IF 9.6
Zhang Ze-Yu,Wang Hai-Bin,Zhang Fei-Fei,Li Jing-Wei,Hu Xin-Zhuo,Yan Si-Wei,Bai Yi-Ming,Zhang Xun,Shen Gu-Rong,Yin Peng-Fei,Yang Jing,Dong Cun-Ku,Mao Jing,Liu Hui,Du Xi-Wen
Electrocatalysis of CO 2 reduction reaction is an effective way to convert CO 2 into high value-added products, but the selectivity of Cu-based catalysts for C 2+ products needs to be improved due to the high energy barrier of C–C coupling. Therefore, a viable catalyst design strategy to decrease energy barrier of C–C coupling should be put forward. Here, a nanocavity-enriched CuPd single atom alloy (CuPd SAA) catalyst is designed to promote C–C coupling process. The faradaic efficiency of CuPd SAA for ethylene and C 2+ reaches 75.6% and 85.7% at − 0.7 V versus reversible hydrogen electrode (RHE), respectively. Based on the results given by in situ characterization, the porous hollow structure dramatically increases the ratio of the linear-bond *CO, thus enhancing the faradaic efficiency for ethylene. Density functional theory (DFT) calculation reveals that the Pd doping can regulate the electronic structure of neighboring Cu atoms to decrease the energy barrier of C–C coupling, further improving the faradaic efficiency. This work provides a new idea for designing catalyst with high selectivity for ethylene. Graphical abstract
研究领域:
材料科学
·
化学
·
电化学
·
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）