JOURNAL OF HAZARDOUS MATERIALS
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2024
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IF 12.2
Ningxuan Xue,Zhaobing Guo,Xinyu Gai,Yiyang Chen,Siyue He,Guanjie Lin,Fengling Liu,Shuai Zhang,Pengxiang Qiu
Ferrate (Fe(VI)) is a widely used water purifier and is easily affected by external factors. Given that the actual water environment conditions are complicated, this study designed an oxygen-doped carbon nitride (CNO) with rich electron sites to explore whether direct electron transfer promotes the degradation efficiency of Fe(VI) for pollutants under visible light. For comparison, we also prepared phosphorus-doped carbon nitride (CNP), which has electron-deficient sites and indirect electron transfer. In the CNO/Fe(VI)/light system, not only more high-valent iron and reactive oxygen species were generated, but also the pollutant degradation rate, reaction kinetics, and electron yield were significantly better than those of the CNP and CN systems, verifying the superiority of direct electron transfer. In addition, CNO showed excellent performance in both actual solar photocatalysis and continuous flow experiments. Therefore, the photocatalysis/direct electron transfer mechanism proposed provides an innovative strategy for improving the application potential of Fe(VI) in the field of pollution control and its industrialization application.
研究领域:
环境科学
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材料科学
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DOI
PubMed
高影响因子
FOOD CHEMISTRY
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2024
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IF 8.5
Hua Wang,Lin Hao,Yaxing Guo,Chun Wang,Qiuhua Wu,Zhi Wang
Porous electron-rich organic frameworks have attracted an increased attention in the adsorption and removal of pollutants due to their abundant electron-rich nitrogen atoms, which can effectively interact with positively charged substance. In this study, a porous electron-rich organic framework (Car-POF) and positively charged amino-functionalized magnetic nanoparticles (Fe 3 O 4 -NH 2 ) were used to construct a magnetic electron-rich Fe 3 O 4 -NH 2 @Car-POF for the enrichment of some phenylurea herbicides from water and milk samples prior to high performance liquid chromatographic detection. The adsorption capacity of Fe 3 O 4 -NH 2 @Car-POF for the phenylureas ranged from 14.93 to 28.83 mg g −1 . The LODs were observed in the range of 0.05–0.20 ng mL −1 and 0.5–1.5 ng mL −1 , and LOQs in the range of 0.17–0.66 ng mL −1 and 1.7–5.0 ng mL −1 for water and milk samples with RSD less than 9.0. The adsorption studies with cationic and anionic dyes revealed that Fe 3 O 4 -NH 2 @Car-POF is favorable for the adsorption of positively charged compounds.
研究领域:
环境科学
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分析化学
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Ye Wang,Yingkui Yan,Huabin Zhang,Xinsheng Peng,Hubiao Huang,Songtao Zhang,Li Shi
The development of unique single-atom catalysts with electron-rich feature is essential to promoting the photocatalytic CO 2 reduction, yet remains a big challenge. Here, a conceptionally new single-atom catalyst constructed from atomically dispersed Ni–P 3 species on black phosphorus (BP) nanosheets (BP-Ni) is synthesized for realizing highly efficient visible-light-driven CO 2 reduction when trapping photogenerated electrons from homogeneous light absorbers in the presence of triethanolamine as the sacrificial agent. Both the experimental and theoretical calculation data reveal that the Ni–P 3 species on BP nanosheets own the electron-rich feature that can improve the photogenerated charge separation efficiency and lower the activation barrier of CO 2 conversion. This unique feature makes BP-Ni exhibit the much higher activity as cocatalyst in the photocatalytic CO 2 reduction than BP nanosheets. The BP-Ni can also be applied as a cocatalyst for enhanced photocatalytic CO 2 reduction after combining with CdSe/S colloidal crystal photocatalyst. The present study offers valuable inspirations for the design and construction of effective catalytic sites toward photocatalytic CO 2 reduction reactions.
研究领域:
材料科学
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催化
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环境科学
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化学
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
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2021
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IF 9.229
Liwei Cheng,Qiaonan Zhu,Jiandong Liang,Mengyao Tang,Yan Yang,Sicong Wang,Puguang Ji,Gongkai Wang,Wenxing Chen,Xiuhui Zhang,Hua Wang
Aqueous zinc-ion batteries (ZIBs) are regarded as a promising candidate for ultrafast charge storage owing to the high ionic conductivity of aqueous electrolytes and high theoretical capacity of zinc metal anodes. However, the strong electrostatic interaction between high-charge-density zinc ions and host materials generally leads to sluggish ion-transport kinetics and structural collapse of rigid cathode materials during the charge/discharge process, so searching for suitable cathode materials for ultrafast and long-term stable ZIBs remains a great challenge. Herein, flexible electron-rich ion channels enabling fast-charging and stable aqueous ZIBs have been demonstrated. Because of the nitrogen-rich conjugated structure of organic phenazine (PNZ) molecules, electron-rich ion channels are formed with the C═N redox centers situated on the channel surface, where zinc ions can transport rapidly and react with active moieties directly. Meanwhile, the π-conjugated systems and inherent flexibility of PNZ molecules can accommodate rapid strain changes and maintain their structural stability during zinc-ion intercalation/deintercalation. Consequently, they exhibit a high capacity of 94.2 mAh g–1 at an ultrahigh rate of 700C (208.6 A g–1) and an ultralong life over 100,000 cycles at 100C, which are superior to those of previously reported aqueous ZIBs. Our work presents a new way for developing ultrafast and ultrastable aqueous ZIBs.
研究领域:
电化学储能
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材料化学
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能源科学
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纳米材料
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电化学
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功能材料
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DOI
高影响因子
Nature Communications
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2021
·Vol. 12
·期 1
·1-9
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IF 14.919
Zhang Lei,Chen Zhe,Liu Zhenpeng,Bu Jun,Ma Wenxiu,Yan Chen,Bai Rui,Lin Jin,Zhang Qiuyu,Liu Junzhi,Wang Tao,Zhang Jian
Electrocatalytic acetylene semihydrogenation is a promising alternative to thermocatalytic acetylene hydrogenation due to its environmental benignity and economic efficiency, but its performance is far below that of the thermocatalytic reaction because of strong competition from side reactions, including hydrogen evolution, overhydrogenation and carbon–carbon coupling reactions. We develop N–heterocyclic carbene–metal complexes, with electron–rich metal centers owing to the strongly σ–donating N–heterocyclic carbene ligands, as electrocatalysts for selective acetylene semihydrogenation. Experimental and theoretical investigations reveal that the copper sites in N–heterocyclic carbene–copper facilitate the absorption of electrophilic acetylene and the desorption of nucleophilic ethylene, ultimately suppressing the side reactions during electrocatalytic acetylene semihydrogenation, and exhibit superior semihydrogenation performance, with faradaic efficiencies of ≥98 % under pure acetylene flow. Even in a crude ethylene feed containing 1 % acetylene (1 × 10 4 ppm), N–heterocyclic carbene–copper affords a specific selectivity of >99 % during a 100–h stability test, continuous ethylene production with only ~30 ppm acetylene, a large space velocity of up to 9.6 × 10 5 mL·g cat −1 ·h −1 , and a turnover frequency of 2.1 × 10 −2 s −1 , dramatically outperforming currently reported thermocatalysts.
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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化学工程
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PubMed
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
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2023
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IF 3.6
Yunxin Sun,Ningning Song,Yanchen Han,Shengtao Ding
Here, we report the regiospecific hydrothiolation of electron-rich thioalkynes with exclusive stereoselectivity facilitated by an organic base, which could proceed exceedingly fast under ambient atmosphere and room temperature, affording β trans addition products in up to nearly quantitative yields. The dual nature of the sulfur atom in attracting and donating electrons is supposed to be pivotal in determining the regio- and stereoselectivity. This system tolerates a wide range of thiols and thioalkynes and shows great potential in polymer synthesis.
研究领域:
有机化学
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材料科学
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DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
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2025
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IF 7.3
Shenghan Gao,Yuting Luo,Bo Li,Wen Cai,Huai Liu,Rui Zhang,Wenlong Jia,Lincai Peng
Modulating the electronic environment of single-atom metal catalysts is a promising yet challenging strategy to optimize their catalytic performance. Herein, electron-rich Ru single atoms were successfully confined within a CoOx matrix (Ru0.6CoOx) through a simple manual grinding-reduction strategy. The resulting Ru0.6CoOx catalyst demonstrated exceptional catalytic activity for the hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF), affording a nearly quantitative DMF yield with an impressive DMF productivity of 210.2 molDMF·mol–1Ru·h–1 at 160 °C. This productivity outperforms most of the noble metal-based catalysts for DMF production. Notably, Ru0.6CoOx also enabled the efficient conversion of HMF to DMF at a low reaction temperature of 120 °C or using a concentrated HMF solution (up to 20 wt %). Experimental studies combined with density functional theory calculations (DFT) revealed that the electronic interaction between the Ru species and CoOx generates electron-rich Ru single atoms, which serve as active sites to boost the H2 activation. Furthermore, the introduction of single Ru atoms was shown to increase the acidity of Ru0.6CoOx, thereby facilitating the cleavage of the C–OH bond during HMF hydrogenolysis. The boosted H2 activation ability and improved acidity of Ru0.6CoOx contribute significantly to its outstanding catalytic performance. This work provides valuable insights into the preparation of electron-rich single-atom metal catalysts for the catalytic hydrodeoxygenation of biomass-derived chemicals.
研究领域:
催化化学
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材料科学
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化学工程
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生物质转化
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密度泛函理论（DFT）
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DOI
高影响因子
DYES AND PIGMENTS
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2020
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IF 4.613
Wei Ma,Yue Wang,Jing Gao,Ru Sun,Jian-Feng Ge
A series of bispyrazolopyridine (BPP) dyes with electron deficient or electron rich aromatic rings were synthesized, and their optical properties were evaluated. Dyes 3a-c connect the BPP unite with electron deficient moieties (pyridine ( 3a ), nitrobenzene ( 3b ), benzonitrile ( 3c )) by a single bond; dyes 3d-e consist of BPP and electron rich moieties (anisole ( 3d ), N,N -diethylaniline ( 3e )). Their optical properties in five organic solvents and water solution were investigated. They show absorption at 310–375 nm and emission at 400–580 nm in organic solvents. Meanwhile, dyes 3a and 3c-d have high fluorescence quantum yield in organic solvents (40%–84%) and aqueous solution (69%–89%), and they also exhibit excellent light stability. The pH-influenced optical properties tests indicate dyes 3a-e show different fluorescence intensities from alkaline (pH = 10.0) to acid condition (pH = 1.0). The protonation of BPP units and aromatic rings was used to explain their emission property, while (TD)DFT calculations were developed to understand the differences in the optical properties.
研究领域:
化学
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材料科学
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光学
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DOI
高影响因子
FUEL
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2025
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IF 7.5
Xiang Tan,Peng Luo,Liya Cao
Hydrodeoxygenation (HDO) is pivotal for upgrading lignin-derived streams into drop-in aviation fuels. Efficient aryl C–O bond cleavage with complete deoxygenation typically requires harsh conditions. Here we report electron-rich Pt nanocatalysts that convert lignin-derived model compounds and lignin oil to jet-range cycloalkanes under notably mild conditions (100 °C, 10 % H 2 /Ar at 0.5 MPa). Alkyl cyclohexanes are obtained in 95.2 % yield from a representative model substrate and 90.5 % from lignin oil. Time-resolved profiling and cascade-kinetics analysis indicate that aryl C–O bond scission is the rate‑determining step. Differential charge density and reaction free‑energy analyses support that increasing electron density on Pt promotes H* activation and lowers the free‑energy change (ΔG) for C–O cleavage, consistent with the enhanced activity. The catalysts exhibit broad substrate scope and reusability. This work provides a practical low-temperature route and an electronic-structure design principle for energy-efficient upgrading of lignin-derived oils to jet-range cycloalkanes.
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高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2025
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IF 9
Yun-Long Gui,Heng Xu,Tong-Mou Geng,Ya-Jie He
Imidazole has a high iodine uptaking capacity thanks to its electron-rich nature, but there are no reports of flexible dibenzimidazole-linked COFs for iodine adsorption. Herein, we present a series of dibenzimidazole-linked COFs, which were formed via Schiff base polymerization of 3,3′- diaminobenzidine (DAB) and 1,2,4,5-benzenetetramine tetrahydrochloride (TAB) with the knots containing ether bonds, NOP–6–CHO and TPT–3–CHO, under different catalytic conditions for the first time (TPT − 3 − CHO + DAB→TDAB, TPT − 3 − CHO + TAB→TTAB, NOP − 6 − CHO + DAB →HDAB, and NOP − 6 − CHO+ TAB→HTAB). TDAB, TTAB, HDAB, and HTAB have large specific areas of 2087, 1912, 2164, and 2001 m 2 g −1 , certain crystallinity and stability. TDAB, TTAB, HDAB, and HTAB showed up to 4.95, 4.86, 5.88 and 6.00 g g −1 iodine adsorption capacities respectively under 77 °C/air conditions, and showed rapid adsorption rates at 25 °C in cyclohexane solution and aqueous solution. The iodine adsorption behaviors conformed to the fitting of the pseudo-first-order model. The plentiful N-heterocycic structure of dibenzimidazole is favorable for electron transfer, which boosts the generating (poly)iodide ions and increases the amounts of iodine adsorbed. For economic reasons, the current novel materials also showed a certain degree of reusability and conserved the iodine capture ability after several regeneration cycles.
研究领域:
材料科学
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环境化学
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吸附技术
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高分子化学
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可持续能源材料
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产品关联
DOI
高影响因子
Science Bulletin
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2022
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IF 20.577
Qi Hao,Qi Tang,Hai-Xia Zhong,Jia-Zhi Wang,Dong-Xue Liu,Xin-Bo Zhang
Single-atom catalysts (SACs) have attracted increasing concerns in electrocatalysis because of their maximal metal atom utilization, distinctive electronic properties, and catalytic performance. However, the isolated single sites are disadvantageous for reactions that require simultaneously activating different reactants/intermediates. Fully exposed metal cluster catalyst (FECC), inheriting the merits of SACs and metallic nanoparticles , can synergistically adsorb and activate reactants/intermediates on their multi-atomic sites, demonstrating great promise in electrocatalytic reactions . Here a facile method to regulate the atomic dispersion of Ni species from cluster to single-atom scale for efficient CO 2 reduction was developed. The obtained Ni FECC exhibits high Faradaic efficiency of CO up to 99%, high CO partial current density of 347.2 mA cm −2 , and robust durability under 20 h electrolysis. Theoretical calculations illuminate that the ensemble of multiple Ni atoms regulated by sulfur atoms accelerates the reaction kinetics and thus improves CO production.
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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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2025
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IF 8.2
Kun Lang,Yuanyingxue Gao,Xudong Xiao,Qi Li,Mingyang Liu,Jianan Liu,Huiquan Gu,Wei Wu,Huiyuan Meng,Baojiang Jiang
Seawater electrolysis offers a sustainable pathway for green hydrogen production, but chloride-induced side reactions, particularly chlorine evolution (ClER), limit the stability and efficiency of catalysts. Based on an interface-engineering strategy, a bifunctional CoP–MXene electrocatalyst was designed and fabricated, in which electrons are transferred from the Ti sites of the MXene support to the adjacent Co active centers of CoP. This directional electron donation modulates the Co electronic structure, generating electron-rich Co sites that effectively suppress Cl– adsorption via electronic repulsion while preserving the OH– reaction pathways through favorable proton–electron coupling. X-ray absorption fine structure (XAFS) spectroscopy, in situ Raman spectroscopy, and density functional theory (DFT) calculations further validate this electron modulation mechanism. In 1 M KOH electrolyte, CoP–MXene achieves a hydrogen evolution reaction (HER) overpotential of only 93 mV at 10 mA cm–2 and an oxygen evolution reaction (OER) current density of 50 mA cm–2 at 346 mV. In alkaline seawater, CoP–MXene exhibits exceptional HER performance (10 mA cm–2 @ 101 mV). Moreover, in an anion exchange membrane (AEM) electrolyzer (at 2 A cm–2 current density), the catalyst maintains over 500 h of stability in seawater with only 8.5% current decay, significantly outperforming the control samples. This study provides a new design strategy for the development of chloride-resistant electrocatalysts, advancing the application of seawater electrolysis technologies.
研究领域:
电化学
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催化
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能量转换
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材料科学
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可再生能源
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表面科学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）