ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Kun Li,Chengjie Duan,Weitao Mao,Dongliang Wang,Yumeng Liang,Wenbo Ye,Guangke He,Xiang Liu
A direct and efficient synthesis of N-methyl-1,2,3,4-tetrahydroquinolines (MTHQs) is achieved through the one-pot reductive N-methylation of quinolines. The SnOx-decorated Pt/Al2O3 (Pt-SnOx/Al2O3) catalyst proves to be highly effective in the transformation from quinolines to MTHQs, using methanol as the exclusive source for hydrogen (H) and methyl (CH3), without the addition of additional bases or additives. Mechanistic and kinetic studies reveal a tandem reaction pathway: (1) the dehydrogenation of methanol, (2) reduction of quinolines to 1,2,3,4-tetrahydroquinolines (THQs), and (3) N-methylation of THQs to MTHQs, with the dehydrogenation of methanol identified as the rate-determining step. Characterization and catalytic performance results demonstrate that SnOx modifies the morphology and electronic properties of Pt-based metal active sites, which dramatically facilitates the cleavage of O–H and less reactive C–H bonds in methanol, and maintains a delicate balance between methanol dehydrogenation and reductive N-methylation of quinolines, thus obtaining a high reactivity for the total transformation.
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Molecular Catalysis
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2024
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IF 3.9
Narina Wang,Chaolumen Bai,Xiaomin Ge,Dan Liu,Agula Bao,Tegshi Muschin,Yong-Sheng Bao
Transamidation of secondary amides via heterogeneous strategy has remained an unsolved problem. Here we report a novel and efficient approach for transamidation and esterification of ubiquitous N -heteroaryl amides with various amines and alcohols that exploits an engineered heterogeneous supported copper nanoparticles catalyst. This method overcomes the difficulty of heterogeneous catalysts, which can only achieve transamidation of primary amide driven by the emission of ammonia gas. A broad diversity of N -heteroaryl amides containing quinolin-2-yl, isoquinolin-1-yl, pyrazin-2-yl and pyridin-2-yl directing groups convert into corresponding α-ketoamides and α-ketoesters using needle-shape copper nanoparticles supported on γ-Al 2 O 3 as heterogeneous catalyst. This environmentally benign, catalyst recyclable and easy-to-handle catalysis methodology will have great application prospects in the pharmaceutical synthesis and biological or chemical industry.
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Journal of the American Chemical Society
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2024
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IF 14.4
Baoxin Ni,Peng Shen,Guiru Zhang,Jiajun Zhao,Honghe Ding,Yifan Ye,Zhouying Yue,Hui Yang,Hao Wei,Kun Jiang
Pt is a well-known benchmark catalyst in the acidic oxygen reduction reaction (ORR) that drives electrochemical O2-to-H2O conversion with maximum chemical energy-to-electricity efficiency. Once dispersing bulk Pt into isolated single atoms, however, the preferential ORR pathway remains a long-standing controversy due to their complex local coordination environment and diverse site density over substrates. Herein, using a set of carbon nanotube supported Pt–N–C single-atom catalysts, we demonstrate how the neighboring N dopants regulate the electronic structure of the Pt central atom and thus steer the ORR selectivity; that is, the O2-to-H2O2 conversion selectivity can be tailored from 10% to 85% at 0.3 V versus reversible hydrogen electrode. Moreover, via a comprehensive X-ray-radiated spectroscopy and shell-isolated nanoparticle-enhanced Raman spectroscopy analysis coupled with theoretical modeling, we reveal that a dominant pyridinic- and pyrrolic-N coordination within the first shell of Pt–N–C motifs favors the 4e– ORR, whereas the introduction of a second-shell graphitic-N dopant weakens *OOH binding on neighboring Pt sites and gives rise to a dominant 2e– ORR. These findings underscore the importance of the chemical environment effect for steering the electrochemical performance of single-atom catalysts.
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Journal of Materials Chemistry A
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2024
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IF 10.7
Shuaipeng Wang,Shengli Zhu,Zhenduo Cui,Zhaoyang Li,Shuilin Wu,Wence Xu,Zhonghui Gao,Yanqin Liang,Hui Jiang
The quest for a cost-effective, high-performance catalyst for hydrogen production from electrolyzed water across a broad pH range holds immense importance. B, N co-doped Mo2C was first synthesized via microwave plasma chemical vapor deposition (MPCVD) for efficient hydrogen production from electrolyzed water. The B, N-Mo2C catalyst demonstrates a requirement of 81 mV in 1.0 M KOH to achieve a current density of 10 mA cm−2. Density functional theory (DFT) calculations revealed that B, N co-doping optimizes the charge transfer between H* and Mo2C, diminishes the excessive hydrogen binding energy of Mo2C, and supports effective and stable hydrogen evolution reaction (HER) conduction in diverse settings. This doping strategy offers a systematic design approach for designing highly active noble-metal-free HER catalysts.
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DYES AND PIGMENTS
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2025
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IF 4.2
Xin-Ke Shao,Lu Fan,Jie-Li Zhou,Kai Wang
The development of novel molecular probes for real-time monitoring of aminopeptidase N (APN) activity is crucial for understanding inflammatory bowel disease (IBD) progression. Here, we present a new probe, HDAPN, a near-infrared (NIR) activatable fluorescent probe based on a hemicyanine scaffold, designed for selective APN detection. Structural characterization confirmed the molecular integrity of the probe, while spectroscopic studies demonstrated its exceptional photostability and response. HDAPN exhibits a remarkable "turn-on" response (720 nm emission) upon APN-mediated cleavage, with outstanding sensitivity (LOD = 0.82 ng/mL) and linearity under physiological conditions. The probe showed minimal cross-reactivity with interferents (e.g., ROS, metal ions, and other enzymes) and successfully detected LPS-induced APN upregulation in RAW264.7 macrophages. In DSS-induced colitis models, HDAPN enabled non-invasive visualization of APN activity, with fluorescence intensity correlating with disease severity (2-fold increase in severe colitis). Comprehensive toxicity evaluations confirmed its biosafety in vitro and in vivo . These findings highlight the potential of HDAPN as a robust tool for studying APN-associated pathophysiology and therapeutic development.
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ACS Catalysis
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2024
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IF 11.3
Xiaohui Leng,Xin Zhou,Lu Ma,Yonghua Du,Ouwen Peng,Zhongxin Chen,Jinhui Pan,Ming-Yu Qi,Jian-Hui Zheng,Yi-Jun Xu,Kian Ping Loh
Visible light induced oxidative C–C and C–N coupling provides a milder alternative to the current synthetic strategies. However, the photochemical C–C coupling of benzylamine and chromoselective C–C/C–N conversion are not widely reported. Herein, we demonstrate that the introduction of indium vacancies in ZnIn2S4 improves the catalytic activity for C–C coupling of benzylamine and imparts a strong chromoselectivity for C–C or C–N coupled products. A high C–C selectivity of ∼80% is achieved with a benzylamine conversion of ∼80%. Mechanistic studies unveil the switchable reaction routes between kinetically favored C–C coupling and thermodynamically favored C–N coupling under specific illumination conditions.
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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Shuwen Zhu,Huiqing Fan,Peizhi Dong,Yuxin Jia,Lin Lei,Yao Su,Yongbo Fan,Weijia Wang
Achieving high sensitivity and reliable detection of trace volatile organic compounds (VOCs) at room temperature remains a significant challenge for metal oxide semiconductor (MOS)-based gas sensors. In this work, we synthesized WO 3 microspheres and PEDOT:PSS@WO 3 (PPW) core-shell heterostructures through a combination of solvothermal treatment and in situ polymerization. The resulting composites were used as active sensing materials for triethylamine vapor detection at room temperature. The PPW-based sensors exhibited excellent TEA sensing performance, which may arise from the synergistic effects of the strong amine affinity of PEDOT:PSS, p–n heterojunction at the PEDOT:PSS/WO 3 interface and the core-shell structure that promotes efficient charge separation and transport. This study demonstrates the significant potential of PPW heterostructures for high-performance, room-temperature sensing of amine vapors and offers a promising strategy for next-generation gas sensor design.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Li Zhang,Jun Cao,Pui Wo Felix Yeung,Hang Jiang,Jianzhong Jiang,Wei Liu,To Ngai
Poly( N -isopropylacrylamide)-based microgels are soft and deformable colloids, which can swell and shrink in response to external stimuli such as temperature or pH, making them suitable for various industries. Herein, poly(styrene- co - N -isopropylacrylamide) microgels with varying softness were synthesized through the doping of different proportions of styrene into their network structure. Rheological tests revealed that the deformability, surface charge, and wettability of microgels were precisely regulated through adjustments to styrene doping levels. As the molar ratio of styrene increased, the range of the linear viscoelastic region regarding stain did not exhibit a consistent change. The microgel suspensions exhibited a pronounced viscous-like behavior, as indicated by their frequency dependence. Additionally, the concentration or volume fraction of microgels significantly influenced the phase distribution in the phase diagram. At lower concentrations, the microgel suspensions typically underwent a colloidal gel-to-liquid-to-glass transition, with the liquid-like regime expanding as the styrene doping level increased. At higher microgel concentrations, the volume phase transition shifted to a direct colloidal gel-to-glass transition, particularly at high styrene levels. This study also revealed a strong correlation between the power-law viscoelastic exponents and the loss tangent during the entire phase transition, offering valuable insights for structure and rheological properties of poly( N -isopropylacrylamide)-based microgels.
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Advanced Science
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2025
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IF 14.1
Siqi Qiu,Hao Wan,Yuechao Yao,Xiao Xu,Zhangjian Li,Yongbiao Mu,Biaolin Peng,Hongliang Wu,Jizhao Zou,Lin Zeng
Iron-nitrogen-carbon (Fe-N-C) materials are promising non-precious metal catalysts for the oxygen reduction reaction (ORR), yet their long-term stability remains a critical challenge due to the dissolution of Fe-based active sites and corrosion of the carbon support. Here, a Fe-Zr dual-atom carbon-based catalyst (Fe,Zr-NC) via a one-step solid-state synthesis method is reported. The introduction of atomically dispersed Zr–N units adjacent to Fe–N 4 centers creates a dual-metal coordination structure that modulates the local electronic environment of Fe and weakens * OH adsorption, which is the rate-limiting step in the ORR process. Density functional theory (DFT) calculations reveal that the Fe–Zr synergy positions the catalyst near the apex of the ORR activity volcano. Extended experimental EXAFS confirms a Fe–Zr distance of ≈3.30 Å, closely matching the theoretical optimum (≈3.39 Å). As a result, Fe, Zr-NC achieves a high half-wave potential (0.891 V vs reversible hydrogen electrode (RHE)) with negligible activity loss over 5000 cyclic voltammetry cycles, outperforming commercial Pt/C. In zinc–air batteries, the catalyst delivers a peak power density of 185.7 mW cm −2 and operates stably for over 453 h. This work highlights the importance of dual-atom synergy in tuning intermediate binding energies and provides design principles for next-generation ORR electrocatalysts.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yifeng Li,Haoxuan Yu,Yuan Ding,Meiting Huang,Yaohui Xie,Peilin Li,Zhihao Wang,Lihua Wang,Liang Chen,Xubiao Luo,Liming Yang
During long–term cycling of LiFePO 4 (LFP) cathodes, the accumulation of surface side reactions usually causes lithium loss and gradual formation of iron phosphate (FP) phase, thus resulting in progressive performance degradation of LFP. Herein, a N doping–assisted regeneration strategy for LFP cathodes is proposed. The inherent carbonaceous impurities in spent LFP are utilized to reconstruct a carbon coating, along with simultaneous N doping by the added urea, thereby enabling the regeneration of high–performance LFP cathodes. The regenerated material (N–doped carbon coated regenerated LFP, abbreviated as RLFP@NC) has a well–maintained crystal structure, which shows an excellent discharge capacity of 106.3 mAh g −1 at a high rate of 5C (1C = 170 mA g −1 ) and a remarkable cycling stability with a capacity retention of 87.2 % after 500 cycles. Theoretical calculations reveal that this enhanced structural stability and improved electrical conductivity are primarily attributed to the presence of N–doped carbon coating. Furthermore, the economic analysis demonstrates that our adopted method is featured with excellent cost–effectiveness and environmental friendliness, offering a viable approach for the green and low–carbon recycling of LFP cathodes.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Ruina Li,Xuwen Li,Qingcheng Liu,Hua Yue,Yang Meng,Yuanyuan Tian
With the continuous advancement of fuel cell technology, the exploration and development of highly efficient non - precious - metal catalysts for the oxygen reduction reaction (ORR) have emerged as a focal point of research. Fe–N–C catalysts have attracted much attention due to their excellent performance and low cost, and coupling single-atom catalysts (SACs) with atomic clusters (ACs) is an effective method to improve catalyst activity. This study used the pyrolysis method to synthesize iron atom catalysts (Fe–N–C SACs) and iron cluster coupled catalysts (Fe–N–C SACs/ACs) on ZIF-8 carbon support. It evaluated the catalyst performance through electrochemical testing. The experimental results showed that the introduction of Fe clusters improved the half-wave potential of the catalyst to 0.399 V, which represented an 8.2 % enhancement compared to the SAC catalyst and reached 87.1 % of that of the commercial Pt–C catalyst, and reduced the Tafel slope to 61.47 mV dec −1 , effectively improving the ORR activity of the catalyst. We constructed FeN 4 single atom catalyst models and FeN 4 /Fe 4 N 6 single atom cluster catalyst models using density functional theory (DFT), analyzed their electronic structures and reaction mechanisms, and revealed the mechanism of action of iron clusters. DFT calculations showed that iron clusters altered the charge distribution of FeN 4 sites, reducing the rate determining step (RDS) (OH desorption) energy to 0.5 eV, which promoted the desorption of products and the re-adsorption of reactants. As a result, the superior electrocatalytic performance of Fe–N–C SAC/AC is attributed to the synergistic effect between iron clusters and single atoms, which is influenced by the coordination environment and provides new ideas for designing efficient ORR catalysts.
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INDUSTRIAL CROPS AND PRODUCTS
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2025
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IF 6.2
Liying Zhang,Hanchen Wang,Zhenghan Cai,Feng Zhu,Biao Huang,Qi-Lin Lu
The construction of hierarchically porous carbon with a rational pore distribution using environmentally benign activators, while simultaneously incorporating heteroatom doping, is crucial for the preparation of electrode materials for supercapacitors. Here, a green one-step method has been developed that utilizes a biomass derivative, chitosan, as the matrix to construct a nitrogen-doped carbon framework, with polyethyleneimine (PEI) for synergistic nitrogen doping and hydrogen bonding interactions to optimize the carbon framework. Phytic acid (PA) is employed as a phosphorus source, activator, and crosslinker to build hierarchical porous carbon containing phosphorus doping, while carboxylated nanocellulose (CNC) is introduced to regulate the uniformity of the pore structure. The resulting HPC exhibits a specific surface area of 939.87 m²/g, a total pore volume of 0.45 cm³ /g, and a high specific capacitance of 350 F/g at a current density of 1 A/g. Furthermore, the HPC supercapacitor assembled at this current density demonstrates an energy density of 18.3 Wh/kg at a power density of 450 W/kg, with a capacitance retention rate of 86 % and a coulombic efficiency of 97 % after 10,000 cycles. Therefore, the approach in this study, which involves the use of PA to activate carbon precursors while incorporating heteroatom doping and adding CNC to promote uniform heteroatom doping, provides valuable insights for the facile, efficient, and green synthesis of biomass-based porous carbon materials, and contributes to energy storage applications.
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