Journal of CO2 Utilization
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2016
·
IF 4.764
Xian-Dong Lang,Yi-Chen Yu,Zheng-Ming Li,Liang-Nian He
Despite recent renaissance of CO 2 chemistry, transformation of CO 2 at ambient conditions remains still of great challenge. In this work, an easily prepared protic ionic liquid e.g. 1,1,3,3-tetramethylguanidinium imidazolide [HTMG][Im] was developed as highly efficient, recyclable and bifunctional catalyst for the carboxylative cyclization of 2-aminobenzonitriles with CO 2 at atmospheric pressure and room temperature. The catalytic protocol was found to be applicable to various 2-aminobenzonitriles bearing electron-withdrawing or electron-donating substituents, affording the corresponding quinazoline-2,4(1H,3H)-diones in moderate to excellent yields. In addition, the catalyst could be conveniently recovered and reused for five cycles with almost consistent activity. Consequently, this process represents an alternative approach for the efficient and greener chemical fixation of CO 2 to afford valuable heterocycles.
研究领域:
有机化学
·
绿色化学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2015
·
IF 2.587
Yujia Xie,Fengyong Zhang,Pingle Liu,Fang Hao,Hean Luo
Direct functionalization of saturated C–H bonds by metalloporphyrin catalysts is among the topical and challenging areas within the chemical industry and synthetic chemistry. In this work, supported CoD(p-Cl)PPCl metalloporphyrin catalysts were prepared and characterized. It has been found that the CoD(p-Cl)PPCl/ZnO catalyst shows better catalytic activity than the supported catalyst (ZrO2, MCM-41, kaolin, Zr(OH)2, and boehmite (BM)) in cyclohexane oxidation with dioxygen. The effects of the reaction pressure, reaction temperature, and reaction time on the catalytic activity were considered by the supported CoD(p-Cl)PPCl/ZnO catalyst. The CoD(p-Cl)PPCl/ZnO catalyst can be facilely recovered and was recycled up to seven times without a significant decrease in catalytic performance. The average cyclohexane conversion and selectivity to KA oil are 10.98% and 84.34%, respectively, and the turnover number is 2.10 × 107.
研究领域:
催化化学
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有机合成
·
工业化学
·
材料化学
·
绿色化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Dandan Yang,Peidong Hong,Yi Hu,Yulian Li,Chengming Wang,Junyong He,Bai Sun,Shuguang Zhu,Lingtao Kong,Jinhuai Liu
CuO particles encapsulated by an irregular polyhedral carbon framework (CuO@C) were prepared via a one-pot polymerization method. The prepared CuO@C exhibited a highly enhanced performance in the activation of peroxymonosulfate (PMS). Our results indicated that the rate constant of tetracycline (TC) degradation was significantly increased by more than 85%, i.e., from 0.021 to 0.147 min −1 , compared with the corresponding value for the bare CuO. TC elimination was completely achieved within 40 min, with the mineralization rate reaching 75.3% in 1 h. In addition, the CuO@C/PMS system exhibited an excellent performance in complex water matrixes containing various inorganic ions. Based on the use of scavengers and spin-trapping electron paramagnetic resonance technology, reactive species including OH, SO 4 − , and 1 O 2 were proposed to be the main oxidants of the CuO@C/PMS system, and the possible intermediates were also fully investigated. Moreover, a catalytic cycle involving Cu + /Cu 2+ /Cu 3+ was proposed. It was also demonstrated that the highly stable CuO@C can be easily recycled and reused. The present study therefore embodies the conceptual design of an excellent catalyst with a persistent stability for the activation of PMS, which may serve as a versatile platform for wider environmental applications.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Xiao-Qian Jin,Jia-Lei Li,Jun-Bin Xiong,Rui Zhang,Chen-Yuan Li,Xue-Ting Wang,Wei-Hong Guo,Da-Chuan Yin
In this work, cross-linked hemoglobin crystals (CLHCs) were synthesized using discarded cow blood as raw material, and palladium nano particles (Pd NPs) was synthesized in situ within its lattice to obtain CLHCs@Pd catalytic used for catalyzing the reduction of Cr(VI). In addition, we investigated the influence of synthesis process on the morphology, loading capacity, and size of Pd NPs, and the results showed that the minimum size of Pd NPs was distributed around 2 nm under any process conditions. The X-ray single crystal diffraction results indicate that the lattice of protein crystals may have a controlling effect on the size of Pd NPs. Subsequently, the mechanism of synthesizing Pd NPs by CLHCs was studied using techniques such as SEM, TEM, FTIR and XPS. Finally, the catalytic activity and cycling performance of Cr(VI) removal by CLHCs@Pd were evaluated. The results indicate that the CLHCs@Pd not only exhibit high catalytic activity for Cr(VI) removal, but also maintain consistent catalytic performance over 20 consecutive catalytic cycles. Overall, this work provides CLHCs@Pd catalysts have the following advantages: (1) small size and uniform dispersion of Pd NPs; (2) High cycling performance and high catalytic activity; (3) Low cost and environmentally friendly preparation process.
研究领域:
环境科学
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材料科学
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纳米技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemistrySelect
·
2025
·Vol. 10
·期 30
·e02557
·
IF 2
Kai Ma,Ziyi Guan,Xuezheng Liang
A novel sulfonated hypercrosslinked aromatic polymer (HCP-SO 3 H) was synthesized through direct condensation of single 1,4-dichloroxylene followed by controlled sulfonation. The rigid aromatic architecture of the porous polymeric material provided abundant anchoring sites for sulfonic groups, endowing the acid catalyst with high acid density (2.6 mmol/g). Characterization revealed an exceptionally high specific surface area (555 m 2 /g) that significantly enhanced substrate accessibility and mass transfer kinetics during catalytic reactions. The water contact angle of 104° indicated the high hydrophobicity of the catalyst. When evaluated in biodiesel production via esterification and integrated esterification–transesterification, HCP-SO 3 H demonstrated remarkable catalytic performance: achieving >98% conversion efficiency for both pure oleic acid and waste frying oil feedstock. The catalyst maintained high activity (>97%) over nine reaction cycles without significant structural degradation. Mechanistic studies identified four critical performance factors: Hierarchical porosity facilitating molecular diffusion, hydrophobicity separated polar by-product from active sites, high-density acid sites ensuring rapid reaction kinetics, andrigid conjugated framework preventing active site leaching. These synergistic characteristics positioned HCP-SO 3 H as a potential heterogeneous catalyst for industrial-scale biofuel production, addressing key challenges in catalyst recyclability and feedstock versatility. Graphical The novel hydrophobic hypercrosslinked polymer based solid acid showed high activity for biodiesel synthesis from both pure oleic acid and waste frying oil feedstock.
✓ 已验证
DOI
高影响因子
ACS Nano
·
2024
·
IF 15.8
Ao Huang,Linglong Kong,Bowen Zhang,Xuefan Liu,Lu Wang,Lifang Li,Jing Xu
Restructuring is an important phenomenon in catalytic reactions. Conversion-type materials with suitable redox potential may undergo in situ electrochemically driven restructurings and induce highly active catalytic sites in a working lithium–sulfur battery. Herein, driven by the electrochemical conversion reaction of BiVO4, a reversible catalytic cycle of Bi/amorphous Li3VO4 (a-Li3VO4) and Bi2S3/a-Li3VO4 heterojunctions is constructed, which targets the oxidation of Li2S and the conversion of polysulfide, respectively. The heterostructures and electrochemically driven size confinement provide abundant sites for shuttle restraining and sulfur conversion. Especially, the p-block Bi and Bi2S3 could dramatically reduce the conversion energy barriers of Li2S and polysulfide by virtue of the p–p orbital hybridization, promoting bidirectional reactions of the sulfur cathode. As a result, the corresponding sulfur cathode possesses a high reversible capacity of 7.5 mAh cm–2 after 120 cycles under a high sulfur loading of 10.3 mg cm–2 with a current density of 0.38 mA cm–2. This study furnishes a feasible scheme to obtain highly effective catalysts for bidirectional sulfur redox by utilizing the electrochemically induced restructuring.
研究领域:
电化学
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储能
·
纳米材料
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催化
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材料科学
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2021
·Vol. 13
·期 21
·4610-4617
·
IF 5.686
Yifei Yang,Linsen Zhou,Jun Chen,Ruizhi Qiu,Yunxi Yao
Graphical Highly dispersed Pt clusters supported on TiN substrates favor the formation of highly reactive dual sites. Molecular O 2 dissociatively adsorbs on the Ti−Ti bridge sites to form titanium oxynitride (TiN x O y ) skin and the oxygen atom binding on Ti sites readily react with the adjacent CO adsorbed on Pt to attain the catalytic cycle. The interfacial synergistic effect between Pt and TiN results in superior performance in the low-temperature CO oxidation. The metal-support interfacial synergistic catalysis allows the competitive reaction steps to occur in close proximity at different sites, thus decreasing the activation barrier and improving the catalytic efficiency. Combining the structural characterization, reactivity assessments and density functional theory (DFT) calculations, it is found that highly dispersed Pt clusters on TiN substrates favor the formation of Pt−TiN interfacial dual sites, which are highly reactive for the low-temperature CO oxidation with an apparent activation energy as low as 38.7 kJ mol −1 , much less than that on the traditional Pt/TiO 2 or Pt/SiO 2 catalysts. At low temperature, the surface sites of Pt are saturated with CO adsorption due to its high adsorption energy and the molecular O 2 dissociatively adsorbs on the Ti sites to form the titanium oxynitride (TiN x O y ) skin with a low barrier of 0.1 eV. The O atoms binding on Ti sites readily react with the adjacent CO molecules adsorbed on the perimeter of Pt clusters to attain a catalytic cycle with a reaction barrier of 0.5 eV. The interfacial synergistic effect between Pt and TiN is the origin of the low temperature CO oxidation activity on the metal-nitride catalysts.
研究领域:
催化
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材料科学
·
化学工程
·
表面化学
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2025
·
IF 4.7
Zongpeng Liu,Shaojian Hu,Qingquan Hao,Rui Ma,Yuning Zhang,Bencheng Wu,Jianhua Zhu
Nowadays, heterogeneous catalytic esterification for synthetic esters production is believed more compatible with the postulates of green chemistry and sustainability goals. In this work, we developed hydrophobic stannous oxide supported on mesoporous silica KIT-6 materials (SnO/KIT-6) via a feasible synthesis and post-grafting modification approach, which served as solid heterogeneous catalysts and then tested in the synthesis of complex polyolester (CPE). The catalytic behaviour of as-prepared catalysts was also systematically investigated and the highest carboxyl conversion ( ca. 95.6%) could be achieved under the optimal preparation conditions within the studied range. The obtained results revealed that Lewis acidity of the tin-based catalysts played a crucial role in esterification conversion efficiency, which varied depending upon the dispersion of different SnO loading. Furthermore, the reusability of the catalyst was evaluated and demonstrated relatively stable catalytic activity for up to five consecutive cycles. Additionally, the possible esterification reaction mechanism of CPE over the modified S-SnO/KIT-6 was also elucidated. The resultant catalysts leveraged full advantage of the unique textural properties and adequate surface hydrophobicity, intensively facilitating the diffusion of large polar molecules and resisting to deactivation from generated water. Collectively, the findings of present study may provide some valuable insights for adopting productive and environmentally benign catalytic processes to synthesize ester-based lubricants in the future.
研究领域:
催化
·
绿色化学
·
材料科学
·
化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Sun Xue,Li Haitao,Song Yajie,Liu Jiaxuan,Ji Pengxiang,Lei Xincheng,zhang Xiangzhi,Liu Qingsong,Li Menglu,Deng Biao,Su Dong,Wang Jiajun
Sodium (Na)-air batteries show significant potential as alternatives to lithium-air batteries due to their high theoretical energy density and the abundant availability of sodium reserves. Nevertheless, the formation of complex products, specifically NaO 2 , Na 2 O 2 , Na 2 CO 3 ·xH 2 O, during the multi-step reactions inevitably raises reconciled potential incompatibility that causes low efficiency and large overpotential. Here, we introduce a cascade electrocatalysis strategy that involves switchable metal and oxygen redox chemistry through electrochemical potential tuning. Leveraging the lithium ion spatial pinning effect, sodium ions trigger in the Na[Li 1/3 Ru 2/3 ]O 2 electrode system to toggle the geometric state at a low electrochemical potential and oscillate among different catalytic states to achieve sequential conversion of complicated multi-step intermediates. The Na[Li 1/3 Ru 2/3 ]O 2 catalyst effectively compartmentalizes the threshold potential that circumvents deactivating or competing pathways while coupling different catalytic cycles. As a result, the sodium-air battery employing this catalyst exhibits long-term reversibility over 1000 cycles with a decent catalysis efficiency exceeding 99%. Our results demonstrate that the cascade electrocatalysis strategy contributes to the design of integrated sodium-air batteries with long-term cycling stability.
研究领域:
储能技术
·
电化学
·
材料科学
·
纳米技术
·
电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Communications Chemistry
·
2025
·Vol. 8
·期 1
·1-11
·
IF 6.2
Wang Min,Luo Xiongfei,Wang Qunying,Strehmel Veronika,Chen Zhijun,Li Shujun,Strehmel Bernd
Valorization of waste for chemical processes addresses a challenging task for the society. Soda lignin ( AL ) available in the pulp industry operated in a photocatalytic cycle CuX 2 / L (X: Br, Cl; L : Me 6 TREN: Tris[2-(dimethylamino)ethyl]amine) and to initiate radical photopolymerization of methyl methacrylate (MMA) with α-bromophenylacetate (EBPA) by exposure at 420 nm. This resulted in poly(methyl methacrylate) (PMMA ) exhibiting a dispersity <1.3 with CuX 2 /L loading of ≲ 52 ppm. Deactivator reduction increased dispersity. MMA, styrene, and benzyl methacrylate successfully served as monomers for chain extension and block copolymerization experiments. This worked with CuX 2 /L ≥ 6.5 ppm, although conventional radical polymerization additionally competed. Adding of sodium pyruvate enabled radical photopolymerization under air. Modification of lignin with an aryl sulfonate group resulted in a one-component photoinitiator. It successfully initiated radical photopolymerization of a monomer mixture of (hydroxyethyl)methacrylate (HEMA) and urethane dimethacrylate (UDMA). Scale-up experiments approved practicability of photo-ATRP.
研究领域:
高分子化学
·
绿色化学
·
光催化
·
材料科学
·
可持续化学
·
工业化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Qi Zhong,Kangdong Wang,Gao Pan,Shuping Peng,Cijun Shuai
CeO2 nanozymes have demonstrated the potential to enhance biological scaffolds with chemodynamic therapy. However, their catalytic efficacy is limited by the slow conversion of Ce4+ to Ce3+ and the lack of substrates like H2O2 and H+. To address these challenges, we adopted a dual-pronged strategy that utilized the plasmonic resonance of Au nanoparticles and their glucose-oxidase mimicry to boost electron and hydrogen transfer. Specifically, we integrated Au/CeO2 nanozymes into poly-l-lactic acid scaffolds via selective laser sintering. This conversion of Ce3+ to Ce4+ in the scaffolds enhanced the reduction of H2O2 to a hydroxyl radical, inducing oxidative stress in tumor cells. The Au nanoparticles played a crucial role in boosting the Ce3+/Ce4+ catalytic cycle by providing both the energy and the catalytic substrates. They recycled Ce4+ back to Ce3+ by exploiting plasmonic-induced hot electrons and catalyzed glucose oxidation to supply H2O2 and H+. Our nanoscale and atomic-scale simulations confirmed that the Au/CeO2 hybrid structure utilized near-field coupling to amplify the plasmonic resonance and the Au–O–Ce bridge reduced the electron transfer barrier. Consequently, the Au/CeO2 scaffold decreased the activation energy from 22.57 to 9.92 kJ/mol. These findings highlight the significant promise of the Au/CeO2 nanozyme scaffold for NIR-enhanced chemodynamic therapy.
研究领域:
纳米技术
·
癌症治疗
·
材料科学
·
生物医学工程
✓ 已验证
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）