JOURNAL OF ORGANIC CHEMISTRY
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2025
·
IF 3.6
Jia-Wei Li,Shuai Shi,Xiao-Hong Chen,Mao-Gui Huang,Yong-Liang Ban,Hui Zhang,Yue-Jin Liu
Direct functionalization of native (N–H) indoles via C–H activation remains a challenge. Herein, we report a salicylaldehyde-promoted cobalt-catalyzed selective C2–H Heck reaction of native (N–H) indoles with both active and unactivated olefins in the presence of free N–H bonds. A series of structurally diverse C2-alkenylated native (N–H) indoles including natural product and drug derivatives were prepared directly and effectively without additional preprotection and deprotection procedures.
研究领域:
有机化学
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药物化学
✓ 已验证
DOI
PubMed
高影响因子
VACUUM
·
2024
·
IF 3.8
Kaiting Yang,Xiongtao Lv,Jingwen Meng,Huiqing Wang,Lin Guo,Xin Li,Fengyun Su,Qing Lan,Zhengdao Li,Wei Wang,Yuwei Guo,Xiaoli Jin,Haiquan Xie
Photothermal catalytic reduction of CO 2 into high value-added C 2 hydrocarbon products is a promising method for efficient CO 2 conversion. However, current photocatalysts still encounter obstacles including limited photoabsorption range, rapid recombination of photogenerated carriers , and inadequate surface active sites. Herein, Bi 4 O 5 Br 2 co-modified with oxygen vacancy (OV) and metal bismuth (Bi) (Bi 4 O 5 Br 2 -OV@Bi) has been prepared to optimize these crucial issues. Bi 4 O 5 Br 2 -OV@Bi delivers a remarkably improvement in CO 2 photothermal conversion, reflecting by the notable increase in C 1 (CO and CH 4 ) and newly generated C 2 (C 2 H 4 and C 2 H 6 ) products compared to pristine Bi 4 O 5 Br 2 . In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) spectrometry reveals that OC−COH* intermediate promotes the C–C coupling for produce C 2 hydrocarbons. This study strengthens the understanding of metal modification and defect engineering for forming C 2 hydrocarbons on bismuth-based photocatalysts .
研究领域:
材料科学
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环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Rui Zhang,Feifei Chen,Haokun Jin,Yong Zhang,Xiaoya Hao,Yingda Liu,Tianming Feng,Xinghua Zhang,Zunming Lu,Weihua Wang,Feng Lu,Hong Dong,Hui Liu,Hui Liu,Yahui Cheng
In Cu-based electrocatalysts, appropriate amount of Cu 0 and high concentration of Cu + are essential for the efficient conversion of CO 2 into C 2+ products. An obstacle of CO 2 electroreduction is the inevitable reduction of Cu + to Cu 0 at cathodic potential. Intermediates confinement is a promising solution to delay Cu + deterioration, in which it is crucial to maintain an appropriate amount of Cu 0 and Cu + species to produce sufficient intermediates to protect most Cu + species. Herein, based on the influence of Cu + /Cu 0 ratio on the reaction process and its feedback, a series of hollow Cu 2 O nanoreactors with different cavity sizes were synthesized to modulate the concentration of intermediates and the coverage degree of Cu + , so as to realize a constant high Cu + /Cu 0 ratio. The optimized hollow Cu 2 O nanoreactors achieved a C 2+ Faradaic efficiency of 70.1 ± 0.2 % at a partial current density of −9.3 ± 0.1 mA cm −2 over 30 h and a large C 2+ -to-C 1 ratio of 9.73. Operando Raman spectra and quasi in - situ Auger electron spectra confirmed that the moderate cavity Cu 2 O nanoreactors led to a full coverage of Cu + and an optimal Cu + /Cu 0 ratio of 8.12:1, which brought the stability of Cu + species and cavity structure, as well as the enhanced C C dimerization.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-12
·
IF 15.7
Song Hui,Sun Kai,Huang Hengming,Ning Shangbo,Wang Shengyao,Wang Zhuan,Weng Yuxiang,Cui Yi,Li Yifan,Wang Xu-sheng,Wang Defa,Liu Lequan,Wang Zhou-jun,Ye Jinhua
The direct photocatalytic oxidation of methane to value-added chemicals has garnered considerable interest in recent years. However, achieving high productivity while maintaining high selectivity at an appreciable methane conversion rate remains a formidable challenge. Here, we present photochemically-triggered and photothermally-enhanced oxidative coupling of methane to multi-carbon C 2+ alkanes over an Au and CeO 2 nanoparticle-decorated ZnO photocatalyst, which exhibits a record-breaking C 2+ production rate of 17,260 μmol g −1 h −1 with ~90% C 2+ selectivity under wide-spectrum light irradiation without a secondary source of heating. Comprehensive characterizations and computational studies reveal that CH 4 activation is a photochemical reaction initiated by ultraviolet light-excited ZnO, and the introduction of CeO 2 substantially enhances the activation of CH 4 and O 2 due to the cooperative interaction between Au and CeO 2 . Concurrently, Au nanoparticles capture visible and near-infrared light to generate localized heating, which greatly promotes the subsequent desorption of produced methyl radical for C–C coupling prior to undergoing further undesired overoxidation.
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Anbang He,Yong Yang,Qiang Zhang,Ming Yang,Qian Zou,Jun Du,Changyuan Tao,Zuohua Liu
Electrochemical reduction of CO 2 to C2 products on Cu-based catalysts provides a promising approach for controlling the global carbon balance and restoring renewable surplus electricity. The enhanced CO 2 adsorption and CO local concentration are beneficial for CO 2 conversion and C2 intermediates formation, promoting the progress of CO 2 utilization. Here, we report a bimetallic MOF-derived Co 3 O 4 -CuO x /C (M-CuCo/C) catalyst constructed with Co 3 O 4 and CuO x sites wrapped in the carbon skeleton, achieving efficient CO 2 activation and C2 generation under low overpotential. The optimized M-CuCo/C catalyst (Cu/Co ratio of 1:2) exhibits a total current density of 19.28 mA/cm 2 at −1.05 (V vs. RHE), which is 8.60 times than that on MOF-derived CuO x /C (M-Cu/C). The highest C2 faradic efficiency (FE) reaches 79.2% (-0.75 V vs. RHE), accompany with a C2 production rate of 275.6 μmol/(g·h). The special nanorods-like morphology assembled by dual sites significantly increases electrochemical surface area and electron transmission rate during eCO 2 RR. The local CO intermediates under real-time electrochemical environment are monitored via rotation ring disk electrode (RRDE) techniques. Combined with in situ infrared measurements and DFT studies, it’s demonstrated that CO 2 could be efficiently converted to CO under low overpotential on Co 3 O 4 sites, forming local CO-enriched environment around neighboring CuO x sites and further accelerating the process of C2 formation.
研究领域:
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
Materials Advances
·
2022
·Vol. 3
·期 12
·4964-4972
·
IF 0
Chong Wang,Chengdeng Wang,Zhihao Xiong,Jiashuai Wang,Wenyuan Zhang,Haofeng Shi,Donghua Wang,Yousong Gu,Zhiming Bai,Yan Gao,Xiaoqin Yan
Electrochemical CO2 reduction reactions (CO2RRs) have been recognized as a promising solution to environmental and energy problems due to their ability to convert intermittent renewable electricity into hydrocarbon fuels and value-added chemicals. Copper has a unique ability to electrochemically reduce CO2 to produce C2+ hydrocarbon products compared to other metals. However, it is still suffering from low Faraday efficiency (FE) limitations for specific products. Herein, we have prepared an Ag-modified Cu/CuO–Ag catalyst with a porous structure via a galvanic replacement reaction method, which reduced CO2 to C2+ products with the FE of 52.5% at −1.1 V (vs. RHE). The experimental results and density functional theory (DFT) calculations show that the addition of Ag in Cu is beneficial to increasing the coverage of *CO on the Cu surface, which can decrease the potential barrier energy of the C–C coupling reaction and favor the generation of C2+ products. The results of this study may be helpful to the design of efficient tandem catalysts for electrochemical CO2 reduction.
研究领域:
能源化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
Soft Matter
·
2012
·Vol. 8
·期 11
·3231-3238
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IF 4.39
Xiaoqiu Dou,Ping Li,Di Zhang,Chuan-Liang Feng
With the development of industry, organic dyes used in printing, textile, plastic, foods, and cosmetics have brought health and environmental issues. A C2-symmetric benzene-based hydrogel with unique layered structure mimicking activated carbon was developed and found capable of the controllable adsorption of 97–99% of certain organic dyes (methylene blue and methyl violet 2B) within two minutes. The adsorption equilibrium of the dyes is in good agreement with the Langmuir adsorption isotherm model. The controllable adsorption of the dyes was confirmed by varying the pH of the medium. The hydrogel's rapid, highly effective, reusable, and controllable adsorption of organic dyes makes it possible to not only adsorb toxic dyes from wastewater, but also be used as potential delivery vehicles for small drug molecules in the field of drug delivery.
研究领域:
环境科学
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
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2021
·
IF 8.271
Yan-Cheng Hu,Ying Li,Ding-Wei Ji,Heng Liu,Hao Zheng,Gong Zhang,Qing-An Chen
C2 prenylated indoles are widespread in a variety of bioactive natural alkaloids. Therefore, the selective installation of prenyl group at C2 position of NH indoles is of great significance. However, the known protocols generally require a multi-step procedure and stoichiometric promoters. Herein we develop a one-step C2 prenylation of NH indole with cheap tert- prenyl alcohol enabled by acid catalysis. Salient features include good regioselectivity, step- and atom-economy, broad substrate scope, and simple catalytic system. The mechanistic investigations demonstrate that both C2 prenylation and C3 prenylation/migration pathways are engaged in the reaction. Notably, this practical strategy can be applied to the late-stage diversification of tryptophan-based peptides and concise synthesis of tryprostatin B.
研究领域:
有机化学
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药物化学
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合成化学
✓ 已验证
产品关联
DOI
高影响因子
ChemElectroChem
·
2021
·Vol. 8
·期 16
·3174-3180
·
IF 4.59
Yunxi Han,Shuaikang Zhu,Shuang Xu,Xiaopo Niu,Zhihong Xu,Rong Zhao,Qingfa Wang
Graphical The structural reconstruction of HKUST-1 on carbon fiber paper and the activity in CO 2 electroreduction is investigated. The HKUST-1 initially reconstructed into highly active 3D nanospheres and then into stable nanobelts after 120 minutes. The 3D nanospheres structure shows the best Faradaic efficiency of C 2 products up to 58.6 %. Metal-organic frameworks (MOFs) have been widely studied for electrochemical CO 2 reduction reaction (CO 2 RR). However, the application of negative potential tends to trigger its structural reconstruction and component alteration. It is of great significance to study the relationship between the structural evolution of MOF-derived materials and product selectivity under the reaction conditions. Herein, we fabricate a HKUST-1 thin film on carbon fiber paper by a facile electrodeposition approach to investigate the variation of CO 2 RR activity with HKUST-1 structural reconstruction. During the CO 2 RR process, the HKUST-1 reconstructs into two structures successively over time: 3D nanospheres composed of numerous small fragments and 3D nano-network composed of cross-linked nanobelts in different directions. The former shows a better catalytic activity due to more active sites, lower charge transfer resistance and higher Cu + /Cu 0 ratio. The optimum Faradaic efficiency (FE) of C 2 products (ethylene and ethanol) reaches 58.6 % at −0.98 V versus reversible hydrogen electrode (RHE).
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2024
·
IF 13
Yi-Ran Du,Xiao-Qiang Li,Xian-Xia Yang,Guo-Yi Duan,Yong-Mei Chen,Bao-Hua Xu
In this study, the copper-nickel (Cu–Ni) bimetallic electrocatalysts for electrochemical CO 2 reduction reaction(CO 2 RR) are fabricated by taking the finely designed poly(ionic liquids) (PIL) containing abundant Salen and imidazolium chelating sites as the surficial layer, wherein Cu–Ni, PIL–Cu and PIL–Ni interaction can be readily regulated by different synthetic scheme. As a proof of concept, Cu@Salen-PIL@Ni(NO 3 ) 2 and Cu@Salen-PIL(Ni) hybrids differ significantly in the types and distribution of Ni species and Cu species at the surface, thereby delivering distinct Cu–Ni cooperation fashion for the CO 2 RR. Remarkably, Cu@Salen-PIL@Ni(NO 3 ) 2 provides a C2+ faradaic efficiency (FE C2+ ) of 80.9% with partial current density ( j C 2+ ) of 262.9 mA cm −2 at −0.80 V (versus reversible hydrogen electrode, RHE) in 1 m KOH in a flow cell, while Cu@Salen-PIL(Ni) delivers the optimal FE C2+ of 63.8% at j C2+ of 146.7 mA cm −2 at −0.78 V. Mechanistic studies indicates that the presence of Cu–Ni interfaces in Cu@Salen-PIL@Ni(NO 3 ) 2 accounts for the preserve of high-valence Cu(I) species under CO 2 RR conditions. It results in a high activity of both CO 2 -to-CO conversion and C–C coupling while inhibition of the competitive HER.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Jiaqi Feng,Yanlin Wang,Guilin Li,Qizhou Xue,Min Wang,Xiaofu Sun,Shaojuan Zeng,Xiangping Zhang
Copper-based catalysts hold promise for electrochemical reduction of CO 2 to multi-carbon (C 2+ ) products, but achieving high selectivity and ampere-level current density remains challenging. A key hurdle lies in stabilizing Cu + species under reducing conditions, which are crucial for C-C coupling reaction. Herein, we modified Cu 2 O with sodium citrate through the coordination interaction between Cu atoms and carboxyl group. In situ spectroscopy analysis and theoretical studies revealed that the modification induced electron transfer from Cu 2 O to the citrate anion, stabilizing Cu + species under reduction conditions. Additionally, the presence of sodium citrate facilitated the hydrogenation of *CO to *CHO, with *CHO being more prone to C-C coupling reactions. Thereby, the as-prepared catalyst showed an C 2+ products Faradaic efficiency (FE) of 88.1 % at − 0.9 V vs reversible hydrogen electrode (RHE) with a C 2+ products partial current density ( j C2+ ) of 825.94 mA cm −2 and maintained over 80 % FE at − 1.1 V vs RHE with j C2+ of 1239.92 mA cm −2 . This work suggests that surface modification of Cu 2 O via carboxyl group is an effective strategy for altering the surface electronic structure of Cu 2 O and regulating the C-C coupling pathway, encouraging the exploration of more carboxyl-containing molecules for modifying copper-based catalysts to further enhance electrocatalytic performance.
研究领域:
电化学
·
催化材料
·
能源转换
✓ 已验证
产品关联
DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2023
·
IF 10.9
Haoyu Sun,Dun Li,Yuanyuan Min,Yingying Wang,Yanyun Ma,Yiqun Zheng,Hongwen Huang
In recent years, Cu-based multi-metallic nanocrystals with controlled elemental distributions have been extensively studied for potential applications as electrocatalysts for CO 2 reduction reaction (CO 2 RR). Modifying Cu electrocatalysts with secondary or additional metals offers a viable approach to manipulate the overall d -band structure which would cause the shift in the d -band center. Such manipulation can affect the surface affinity of Cu towards key intermediates and thus the following catalytic pathway. Apart from endeavors to adjust the electronic structure, morphological engineering provides effective avenues to enhance the electrocatalytic performance of CO 2 RR. In contrast to quasi-spherical particles with irregular shapes, a 3D-assembled porous structure utilizing 2D nanosheets as building blocks offers advantages such as maximizing surface atom exposure and creating numerous diffusion channels and reactive sites for intermediates formed during catalysis. Yet, it is technique challenging to construct such type of nanoarchitecture via a rationally-design synthetic routes and traditional stepwise self-assembling strategy is time-consuming and lack of versatile control over the structural parameters of resulting products. Therefore, it holds significant value to develop a synthesis method capable of yielding high-purity formations of unique nanostructures. These structures should possess accurately controlled elemental compositions and electronic configurations, and establish a potential correlation between structural benefits and enhanced electrochemical performance in CO 2 RR. Herein, we report the controlled synthesis of palladium-copper-silver (Pd-Cu-Ag) nanocrystals with rationally-designed two-dimensional (2D)-three-dimensional (3D) hybrid architectures and validated with the promising use for electrochemical CO 2 reduction (CO 2 RR). The synthetic procedure includes the conversion of Au@Cu x O nanospheres into CuAg hierarchical nanoflowers (HNFs), as directed by the capping agent octadecyltrimethyl ammonium chloride. Interestingly, the nanosheets are formed in situ as the building block. Following galvanic replacement reaction between CuAg HNFs and Na 2 PdCl 4 removes Ag and Cu, introduces zero-valent Pd, and creates abundant pores on the nanosheets. These CuAg-based products are tested as CO 2 RR electrocatalysts, in which the Pd 0.7 Cu 40.0 Ag 59.7 PHNFs displayed the optimized performance in terms of C 2+ products selectivity (69.5%) and C 2+ partial current density (−349.1 mA·cm −2 ). As revealed by density functional theory (DFT) simulations, PdAgCu surface has distinct electronic property, which lower the reaction barrier for C-C coupling, protruding the exceptional advantage of the Pd doping towards CuAg electrocatalysts for CO 2 reduction. The present study offers a straightforward approach to fabricate hierarchical multi-metallic nanostructures with the porous nanosheet as building block, and validates its structural advantage in electrocatalysis, shedding light on the rational design of efficient CO 2 RR catalyst. Download: Download high-res image (72KB) Download: Download full-size image
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
DOI
高影响因子
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