NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Xiang Gao,Jiajia Zhao,Hao Song,Xintong Zhou,Yuehua Deng,Jiali Liu,Yanrui Li
Graphitic carbon nitride (CN), a promising photocatalyst for CO2 reduction, suffers from inefficient light harvesting and sluggish charge separation dynamics, which severely restricts its application. Ionic liquids (ILs) have been used for the assisted preparation of photocatalysts, thus effectively altering their geometric and electronic properties. Herein, the 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim]PF6) IL was introduced as a modifier to successfully construct a P- and F-co-doped porous CN catalyst via simple calcination of the IL and urea without any organic solvents and templates. The optimized catalyst exhibited an enhanced photocatalytic activity for CO2 reduction via gas–solid mode under visible light irradiation, achieving CO and CH4 evolution rates of 39.9 and 2.63 μmol g−1 h−1 (CO selectivity of 94%), which were 7.8 and 4.8 times higher than those of pristine CN, respectively. PFCN also demonstrated excellent reusability and stability. Comprehensive characterization revealed that the strategy of doping of P and F atoms significantly enlarged the surface area, improved CO2 adsorption, broadened visible-light harvesting, and accelerated charge transfer and separation efficiency. This work highlights the potential of ILs as multifunctional agents for designing high-performance doped CN photocatalysts.
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高影响因子
ENVIRONMENTAL RESEARCH
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2025
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IF 7.7
Li Song,Weiguo Zhang,Quan Liu,Xiao Zhang,Fuqiang Liu,Aimin Li
Various organic acids commonly coexist with Cr(VI) in wastewater. However, direct electron transfer between Cr(VI) and electron-rich organic acids is typically slow. Current Fe-based mediators primarily operate through the aqueous Fe(III)/Fe(II) cycle, which faces challenges in achieving efficient Fe recycling. To address the efficient removal of Cr(VI) and sodium citrate (Cit) composite pollutants (Cr(VI)-Cit), iron-loaded carbon nitride composites (Fe/CN) were synthesized via a combined loading-calcination approach. Crucially, coordination between carboxylate groups of Cit and undercoordinated Fe sites on Fe/CN formed photoactive complexes, effectively stimulating ligand-to-metal charge transfer (LMCT). This significantly enhanced the solid-phase Fe(III)/Fe(II) cycling efficiency, leading to a markedly increased Cr(VI) reduction rate constant ( k ) of 0.213 mg/(L·min). Furthermore, coordination with the N-rich matrix effectively inhibited Fe leaching, resulting in a post-reaction total Fe concentration below 0.5 mg/L. The formation of a Cr(VI)-Fe-Cit ternary cyclic complex effectively lowered the activation energy for Cr(VI) reduction by 81.3% compared to pristine CN. In the dark, intramolecular electron transfer within this complex generated Fe(II)-Cit species with a low electrode potential. Under irradiation, the photoactive Fe(III)-Cit complex generated Fe(II) via LMCT to reduce Cr(VI); concurrently, photogenerated electrons (e - ) and superoxide radicals (·O 2 - ) also contributed to Cr(VI) reduction. Reusability tests showed Fe/CN retained ∼90% Cr(VI) removal efficiency from actual wastewater over 5 cycles, demonstrating good stability under realistic conditions. This study provides valuable insights for the cost-effective and efficient remediation of Cr(VI)-organic acid complexes in real wastewater.
研究领域:
环境科学
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材料工程
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化学修复
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无机化学
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水处理技术
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DOI
PubMed
高影响因子
Journal of Materials Chemistry A
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2025
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IF 9.5
Qing Cheng,Yuqi Zhang,Yingying Cao,Peihao Dou,Long Liu,Yanqiang Zhang
Ionic liquid-H2O2 is a green hypergolic propellant system, and the poor self-ignition hinders its application. Herein, the stable zero-valent catalyst Cu nano-particle with twin boundaries (T-Cu) was synthesized. As the twin boundary regulates the electron micro-environment of the T-Cu surface, the electron transfer from the d electrons of Cu atom to the σ* anti-bonding orbital of H2O2 is intensified to create ·OH and ·OOH. The resulted free radicals possess strong oxidizing ability, and react violently with [BMIM]N(CN)2 to achieve a rapid ignition with the delay time as low as 25 ms. This work provides an effective way to get excellent ignition performance, and promotes the application of Ionic liquid-H2O2 green hypergolic propellants.
研究领域:
材料科学
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推进剂工程
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催化化学
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DOI
高影响因子
JOURNAL OF CATALYSIS
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2017
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IF 6.844
Lingfeng Shen,Shanjun Mao,Jianqing Li,Mingming Li,Ping Chen,Haoran Li,Zhirong Chen,Yong Wang
This work highlights a novel hybrid catalyst, intermetallic PdZn on CN@ZnO (PdZn/CN@ZnO), which serves as a highly efficient heterogeneous catalyst for semihydrogenation of 2-methyl-3-butyn-2-ol utilizing water as the solvent. Compared with intermetallic PdZn on ZnO (PdZn/ZnO), PdZn/CN@ZnO displays almost sixfold higher TOF while retaining high selectivity. It is assumed that the introduction of biomass-derived hydrophilic nitrogen-doped carbon into the ZnO helped to promote catalyst dispersion in aqueous media, ensuring better mass transfer. Further experiments and theoretical calculations showed that from Pd particles to intermetallic PdZn, the decrease of corner and edge Pd atoms might be a factor leading to the improvement of selectivity. Recycling experiments demonstrated that the PdZn/CN@ZnO catalyst could be reused at least eight times without significant decrease in activity or selectivity. Furthermore, when applied to industrially relevant alkenols that are building molecules for the production of vitamin E, the present catalyst still offered excellent performance. It is expected that the present catalytic system will demonstrate its high potential for practical production of vitamin E.
研究领域:
催化化学
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材料科学
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有机合成
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DOI
高影响因子
Results in Physics
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2017
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IF 0.946
Lang Yang,Feifei Jia,Bingqiao Yang,Shaoxian Song
The adsorption of gold cyanide complex ion (Au(CN) 2 − ) on graphene oxide-polyethylenimine hydrogel (GO/PEI hydrogel) from gold cyanidation has been studied to explore the possibility of the application of GO/PEI hydrogel in gold cyanidation process for extracting gold from ores. The adsorption was carried out in artificial Au(CN) 2 − aqueous solution with GO/PEI hydrogel as adsorbent. The experimental results, as well as IR, XPS and SEM−EDS, have shown that GO/PEI hydrogel exhibited a high adsorption capacity and a fast adsorption rate of Au(CN) 2 − , suggesting that GO/PEI hydrogel might be a good adsorbent for the recovery of Au(CN) 2 − . The adsorption of Au(CN) 2 − on GO/PEI hydrogel obeyed the Langmuir isotherm model and fitted well with the pseudo second order model. The good recovery of Au(CN) 2 − was largely related to the porous structure, large specific surface area, as well as the oxygenous functional groups on the surface of GO/PEI hydrogel.
研究领域:
材料科学
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环境工程
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化学工程
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DOI
高影响因子
MICROCHEMICAL JOURNAL
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2024
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IF 4.9
Meishuo Bao,Liang Zhang,Rongsheng Xiao,Xingang Wang,Zheqin Dai,Wuxiang Zhang,Jiansheng Li
The presence of resorcinol (RS) in water contaminated with pollutants may engender environmental and ecosystem risks. In this study, we developed rapid and efficient colorimetric methods for the on-site quantitative determination of RS. Specifically, a synthetic nanozyme composed of nitrogen-doped carbon-coated cobalt-iron (CoFe@CN) was utilized to initiate the oxidation reaction of 3,3′,5,5′-tetramethylbenzidine (TMB) with the activator of peroxymonosulfate (PMS). Compared to the activator of hydrogen peroxide (H 2 O 2 ), PMS demonstrated a sixfold enhancement in catalytic efficacy, markedly elevating the detection performance. Density Functional Theory calculations indicate that RS can serve as a reducing agent for oxTMB, confirming the theoretical feasibility of this process. A linear relationship between inhibition rate (IR %) of RS concentration and absorbance was established and the colorimetric analysis revealed a linear relationship between RS concentration and gray scale values over the range of 0–45 μM, with a detection limit of 3.39 μM. Furthermore, smartphone-based analysis of color images allows for on-site quantitative analysis of RS concentration, leveraging portability and real-time detection capabilities. This study provides pioneering analytical support for on-site water quality monitoring within the ecological environment.
研究领域:
环境科学
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分析化学
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DOI
高影响因子
Science Bulletin
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2022
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IF 20.577
Zhuwei Li,Shi Qiu,Yurou Song,Shiyu Huang,Junfeng Gao,Licheng Sun,Jungang Hou
Photoredox catalysis has become an indispensable solution for the synthesis of small organic molecules. However, the precise construction of single-atomic active sites not only determines the catalytic performance, but also avails the understanding of structure–activity relationship. Herein, we develop a facile approach to immobilize single-atom Ni sites anchored porous covalent organic framework (COF) by use of 4,4′,4″-(1,3,5-triazine-2,4,6-triyl)trianiline and 2,6-diformylpyridine (Ni SAS/TD-COF). Ni SAS/TD-COF catalyst achieves excellent catalytic performance in visible-light-driven catalytic carbon–nitrogen cross-coupling reaction between aryl bromides and amines under mild conditions. The reaction provides amine products in excellent yields (71%–97%) with a wide range of substrates, including aryl and heteroaryl bromides with electron-deficient, electron-rich and neutral groups. Notably, Ni SAS/TD-COF could be recovered from the reaction mixture, corresponding to the negligible loss of photoredox performance after several cycles. This work provides a promising opportunity upon rational design of single-atomic active sites on COFs and the fundamental insight of photoredox mechanism for sustainable organic transformation.
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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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Fang He,Hubo Yuan,Huayan You,Zhenxing Wang,Shaoqin Peng,Yuexiang Li
Building carbon nitride (CN)-based core shell heterostructures is an effective strategy to enhance the photocatalytic performance and stability by optimize the interface area and protect the CN core, respectively. Moreover, by fabricating the porous structures in core shells can further optimize the light absorption, charge separation, and mass transfer. Herein, we have constructed porous C-PDA–CN–ms core-shell heterostructures through a facile green molten salt (ms) sculpture the polydopamine (PDA) derived carbon (C-PDA) shells with CN core. In which, the C-PDA-CN core-shells arise from in situ polymerization of dopamine (DA) on the surface of melamine to form PDA@melamine coatings followed by thermal polycondensation . The molten salts at high-temperature act as a green fluid immersing in and out of C-PDA-CN core-shells to further produce porous structures. The 1 wt% C-PDA–CN–ms with porous core-shell structures display photocatalytic H 2 evolution rate of 3830 μmol h −1 g −1 , which is 20.8 times enhancement of 1 wt% C-PDA-CN core-shells, even 73.6 times higher than that of pristine CN. It reveals that the porous and core-shell heterostructures endow C-PDA–CN–ms enhanced light absorption, various charge transport channels for improved charge carrier separation and transfer, contributing to the superior photocatalytic H 2 evolution performance. Our work opens a new window for the green construction of porous core-shell heterostructures of CN-based photocatalysts .
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Xuan Miao,Binbin Wang,Huitao Fan,Peng Zhang,Shiqiang Bai,Weisheng Liu
Semiconducting photocatalysts' electronic configuration significantly impacts their band gaps, charge carrier transport properties, and photocatalytic activities. Boron-doped tremella-like hierarchical CN and ultrathin Co phthalocyanine (CoPe) heterojunction (B 1.5 HCN-Co 0.5% ) formation via strengthened H-bonding interfacial connection possess excellent photocatalytic activities in water where the small amounts of catalysts exhibit a high photocatalytic H 2 evolution activity with H 2 evolution rate of 17818.82 μmol h −1 g −1 under simulated sunlight and 5558.81 μmol h −1 g −1 under visible light (≥420 nm). According to detailed characterization, the unique tremella-like hierarchical structure with abundant mesopores shortens the charge diffusion length. At the same time, incorporating CoPe improves the charge transport properties of B 1.5 HCN achieving effective spatial separation, which is primarily responsible for the improved performance. Both a significant amount of experimental data and theoretical calculations demonstrated the critical role of boron-doped and CoPe in photocatalytic H 2 evolution. Heteroatom doping and heterojunction construction are essential in rationally regulating band structure to construct more efficient CN-based photocatalysts.
研究领域:
材料科学
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能源化学
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光催化
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Yiqun Chen,Xiaori Huang,Dedong Sun,Hongchao Ma,Guowen Wang,Chun Ma,Jun Hao
In this study, the Fe 3 O 4 /Co 3 [Co(CN) 6 ] 2 composite catalyst was synthesized by co-precipitation method. The morphology and the structure of Fe 3 O 4 /Co 3 [Co(CN) 6 ] 2 composites were characterized by XRD, FTIR, SEM, TEM, EDS, XPS, VSM. The results showed that the removal rate of RhB (10 mg/L) reached 99.5% in 40 min in the 0.4-Fe 3 O 4 /Co 3 [Co(CN) 6 ] 2 (200 mg/L) + PMS (50 mg/L) system with a pseudo first-order degradation rate constant (k) of 0.121 min −1 , which is nearly 2.16 times of that (0.0561 min −1 ) in the Co 3 [Co(CN) 6 ] 2 + PMS system and 18.9 times of that (0.0064 min −1 ) in the Fe 3 O 4 + PMS system. The observed synergistic catalysis between Fe 3 O 4 and Co 3 [Co(CN) 6 ] 2 in Fe 3 O 4 /Co 3 [Co(CN) 6 ] 2 enhanced the degradation of RhB. The electron paramagnetic resonance (EPR) analysis and quenching experiment indicated that SO 4 − and OH played important roles in the degradation process of RhB. A synergistic catalytic mechanism of PMS activation by Fe 3 O 4 /Co 3 [Co(CN) 6 ] 2 , which mainly involves the enhanced Co 2+ /Co 3+ cycle by Fe 2+ donated electrons, was proposed. In summary, owing to its easy preparation, excellent catalytic activity, and reusability, the Fe 3 O 4 /Co 3 [Co(CN) 6 ] 2 composite catalyst is a good candidate for remediation of contaminated water.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
ACS Sensors
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2018
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IF 5.711
Jia-Dong Zhang,Lei Lu,Xiu-Fang Zhu,Li-Jing Zhang,Shan Yun,Chuan-Song Duanmu,Lei He
In this work, we developed an innovative closed bipolar electrode (BPE)-electrochemiluminescence (ECL) sensing strategy with generality for target detection. Based on charge balance and 100% current efficiency between the closed BPE poles and the driving electrodes, one of the driving electrodes in one cell of the closed BPE system was employed as ECL sensing surface to reflect the target on the BPE pole in the opposite cell. Compared with traditional BPE-ECL sensing method, which in general adopted the anodic ECL reagents such as Ru(bpy)32+ and its coreactant on one pole (anode) to reflect the target (occurring reduction reaction) on the other pole (cathode), the difference was that the targets occurring oxidation reaction could be detected by the anodic ECL reagents based on this strategy. To verify the feasibility of this strategy, the detection principle was stated first, and Fe(CN)64– as model target at anodic BPE pole were detected by anodic ECL reagents (Ru(bpy)32+ and TprA) on the driving electrode first. The ECL signals showed good performance for target detection. By changing the size and the material of the BPE pole where the targets were located, the detection of l-ascorbic acid (AA), uric acid (UA), and dopamine (DA) as other model targets with higher detection limit were accomplished. Visual and high-throughput detection of AA, UA, and DA were also successfully realized by an array of the closed BPE system. This closed BPE (array) system is an effective supplement of traditional BPE-ECL sensing and could greatly expand the scope of the detection target.
研究领域:
分析化学
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生物传感
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电化学
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DOI
PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2019
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IF 6.393
Tingyan Shi,Zuorui Wen,Lijun Ding,Qian Liu,Yingshu Guo,Caifeng Ding,Kun Wang
A novel photoelectrochemical (PEC) aptasensor for diclofenac detection, based on visible/near-infrared (vis/NIR) light-responsive vanadyl-phthalocyanine/graphitic carbon nitrid nanosheet (VOPc/CN) nanocomposites, was successfully fabricated. In this work, the first coupling of CN and VOPc with a facile solution–phase method was prepared and applied to PEC sensing. The UV–vis diff ;use reflection spectra (DRS) indicated that VOPc is an excellent photosensitizer when applied to the surface of CN. It promoted CN light absorption to the visible-NIR region, which greatly enhanced the light excitation capability. The PEC signal of the VOPc/CN nanocomposites improved 2.7 and 12.42-fold compared with pure VOPc and CN, respectively, indicating that VOPc/CN nanocomposites have good photoelectric activity and enhanced photo-to-current conversion efficiency. As a result, VOPc sensitized CN was introduced as a covalent immobilizing PEC aptasensor for the sensitive and selective determination of diclofenac (DCF). Under optimal conditions, the fabricated PEC biosensor exhibited good PEC performances with high sensitivity, a low detection limit of 0.03 nM (S/N = 3) and a wide linear response, in the range of 0.1-500 nM. This was due to the specific interaction between DCF and the aptamer. It is concluded that VOPc/CN nanocomposites are potentially promising photoactive materials for applications in PEC biosensors, as well as for photocatalysis and other related fields.
研究领域:
分析化学
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环境科学
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生物医学工程
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DOI
高影响因子
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