CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Juejin Teng,Min Wang,Wenwen Zhou,Lina Geng,Yilin Wang,Mingbo Wu,Zhongtao Li
Atomic phosphorus doping creates Lewis-base “proton pump” sites that coordinate interfacial water, dramatically lower the water dissociation barrier (0.87 → 0.05 eV). • This targeted acceleration of the rate-determining step boosts the peak power density of Zn–air batteries to 183 mW·cm -2 . • Increases the open-circuit voltage and broadens the operational voltage window. Development of Fe-NC catalysts is fundamentally challenged by their performance decay in acidic media, originating from insufficient proton-coupled electron transfer kinetics and irreversible iron leaching. Herein, we transcend conventional electronic structure modulation by introducing a local interfacial pH tailoring strategy via atomic phosphorus doping. The incorporated P species, serving as Lewis-base sites, function as efficient “proton pumps”. They actively coordinate with interfacial water molecules via lone-pair electrons, which not only enhances H 2 O adsorption but also significantly weakens the O H bond, drastically reducing the water dissociation energy from 0.87 to 0.05 eV. This triggered water activation creates a unique proton-enriched interfacial microenvironment at the catalyst interface while maintaining an alkaline bulk electrolyte, a phenomenon directly visualized by in-situ Raman spectroscopy. The accelerated local proton supply promotes the rate-determining *OOH formation step, while the modulated electronic structure concurrently stabilizes the Fe-Nₓ centers, suppressing Fe dissolution to a remarkably low level. When deployed in a Zn-air battery, this synergistic mechanism enables the Fe-P-NC cathode to achieve a record-high power density of 183 mW·cm −2 . This work underscores the profound potential of active interfacial microenvironment engineering in breaking the activity–stability trade-off for advanced electrocatalysis.
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Yue Long,Gang Wang,Li Xiao,Hang Xu,Weikui Li,Zezhuan Jiang,Zhenzhen Li,Chaoting Wang,Zhukang Zhang,Cheng Li
Dopant-free poly(3-hexylthiophene) (P3HT) has attracted increasing interest as a stable and solution-processable hole-transporting layer (HTL) for perovskite solar cells (PSCs), yet its relatively weak interfacial contact and limited hole-extraction capability remain major constraints on device efficiency. Here, we demonstrate an effective interfacial engineering strategy using two π-conjugated molecules, triphenylamine (TPA) and 4,4′,4″-tricarboxytriphenylamine (TCTA), to simultaneously regulate the perovskite/P3HT interface and suppress interfacial defects. The benzene-ring frameworks of TPA and TCTA enable strong π–π stacking interactions with the thiophene units of P3HT, improving molecular ordering and facilitating more efficient hole transport. Meanwhile, the carboxyl groups in TCTA provide robust coordination with undercoordinated Pb2+, leading to superior defect passivation and more favorable energy-level alignment at the interface. As a result, TCTA-treated devices exhibit significantly enhanced charge extraction, reduced nonradiative recombination, and improved operational stability. Benefiting from these synergistic effects, the power conversion efficiency of dopant-free P3HT-based PSCs is boosted from 12.66% to 17.17% and 19.68% for TPA- and TCTA-modified devices, accompanied by markedly improved moisture stability and long-term durability. This work provides a promising molecular design principle for constructing high-performance and stable dopant-free P3HT-HTL–based PSCs.
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CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Tiantian Qu,Xinran Duan,Zhuowei Ma,Fusheng Liu,Jingjing Ma,Kunqi Gao,Mengshuai Liu
Several phenylpyridine- and phenyl-based hypercrosslinked polymers (HCPs) were prepared via a one-step Friedel-Crafts polymerization and used as catalysts for the cycloaddition reaction between atmospheric CO 2 and epoxides to produce cyclic carbonates. The structural characteristics and catalytic activity of different HCP catalysts were compared, while the recycling performance and universality to various substituted epoxides were investigated. The as-prepared catalysts exhibited regular pore structure and high specific surface area (1133 m 2 /g). Under the synergistic effect of tetrabutylammonium iodide (TBAI), the optimized TPA-HCP-Py efficiently converted atmospheric CO 2 into cyclic carbonates with good to excellent product yields. Furthermore, the TPA-HCP-Py catalyst was easy to recover, and no significant changes were observed after reusing for five times, which demonstrated its excellent recycling performance. The interactions between different active sites and reactants in the TPA-HCP-Py/TBAI catalytic system were investigated by DFT calculation, revealing the catalytic reaction mechanism and providing valuable guidance for developing new multifunctional catalysts.
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ACS Applied Polymer Materials
·
2026
·
IF 5.2
Rui Zhang,Zhengfeng Xie,Yujie Hu,Jie Li,Hong Liao,Junjie Gao,Wei Shi,Chuxiang Zhou
The complexity of pollutants in water, including endocrine-disrupting chemicals, dyes, and antibiotics, poses a challenge to existing water treatment agents. Therefore, we successfully cross-linked tris(4-formylphenyl)amine (TFPA) onto β-cyclodextrin (β-CD) to synthesize a β-cyclodextrin polymer (TFPA-N-β-CD). This unique adsorbent provides essential adsorption properties from each of its components: β-CD offers a cavity structure and hydrophilic groups capable of removing organic micropollutants through host–guest interactions, while TFPA not only constructs a three-dimensional network structure to enhance the specific surface area (63.68 m2/g) but also provides adsorption sites. In single-component systems, the adsorption of bisphenol A (BPA), methylene blue (MB), and tetracycline (TC) follows the pseudo-second-order kinetic model and the Sips adsorption isotherm model. The maximum adsorption capacities are 164.73 (BPA), 272.03 (MB), and 33.89 mg/g (TC). In binary system mixed adsorption, each pollutant still maintains significant adsorption capacity, with adsorption capacity ratios (Rq) greater than 0.80. This reveals the different mechanisms behind the adsorption of TFPA-N-β-CD. During the adsorption of BPA, host–guest interactions dominate, while electrostatic forces are stronger than hydrophilic and inclusion interactions in MB adsorption, and hydrophilic interactions play a dominant role in TC adsorption. Additionally, after 10 consecutive adsorption–desorption cycles, the adsorption capacity of TFPA-N-β-CD for the target pollutants was maintained at over 55% of its initial value, demonstrating its excellent cycling stability and potential for reuse. These characteristics make it highly promising for the treatment of complex real wastewater.
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ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
Ke Min,Yong Li,Yue Lin,Xuezhi Yang,Zigu Chen,Bo Chen,Ming Ma,Qian Liu,Guibin Jiang
Soot, mainly derived from incomplete combustion of fossil fuel and biomass, exists ubiquitously in different environmental matrixes. To study the detrimental effects of soot on climate, air quality, and human health, accurate quantification of soot is an important prerequisite. However, until now, quantification of soot in environmental media, especially in carbonaceous media, is still very challenging. Here, we report a matrix-free laser desorption/ionization mass spectrometry (LDI-MS) method for in situ imaging of soot particles in size-segregated aerosol samples collected on filter membranes. A series of round-shaped sample spots in filter membranes were selected and subjected to MS imaging analysis, enabling direct in situ quantification of soot without solvent extraction or separation. Especially, the MS imaging with serial sample spots can overcome the problems of sweet-spot in LDI-MS and inhomogeneous distribution of soot in the filter membrane, thus greatly improving the precision of quantification. The limit of detection of soot was 4 ng/m2 and the recovery was 84.4–126%. By using this method, we found that a higher soot content was present in larger-sized particulate matter than smaller-sized particles, suggesting that aerosol soot was mainly derived from primary emission sources. Furthermore, this method also shows the potential to analyze nitrate and sulfate species in PM2.5. To the best of our knowledge, it is the first method capable of simultaneous analysis of inorganic salts and soot in air samples. It represents a novel strategy for in situ quantification of aerosol soot with the advantages of high specificity, high sensitivity, separation-, solvent- and matrix-free.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jingjing Wang,Jinyang Feng,Chuanfu Wei
In the present study, molecularly imprinted polyaniline was immobilized on Fe 3 O 4 /ZnO composite by surface imprinting technique. The obtained molecularly imprinted photocatalyst was used for selective degradation of amoxycillin under visible light irradiation. The presence of Fe 3 O 4 not only endowed the photocatalyst with magnetic separation feature but also enhanced visible light harvesting ability. Compared with Fe 3 O 4 /ZnO composite, photocatalytic performance of the molecularly imprinted photocatalyst was significantly improved because polyaniline could form a heterojunction with ZnO to enhance photocatalytic performance. The molecularly imprinted photocatalyst displayed better photocatalytic efficiency and selective photodegradation activity towards amoxycillin than the non-imprinted photocatalyst, because the photodegradation reaction could take place not only on surface of the photocatalyst but also in imprinted cavities for the molecularly imprinted photocatalyst, while the photodegradation only occurred on surface of the non-imprinted photocatalyst. Active species capture experiments showed that .O 2 - and h + played a crucial role in the degradation of amoxycillin. The current research provided new insight for fabrication of molecularly imprinted photocatalyst with selective degradation ability for organic pollutants.
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TALANTA
·
2023
·
IF 6.1
Peijiang Wang,Shanshan Jiang,Jun Zeng,Yuewen Huang,Bin Song,Bin Wang
Luminescent metal-organic frameworks (LMOF) with ligand-modified are a promising strategy to be applied to fabricate chemical sensors. Herein, a novel Co (II) metal-organic framework (Co-MOF), namely Co [(NTB) bpy] (NTB = 4,4′4″-tricarboxylic acid triphenylamine, bpy = 4,4 ′-bipyridyl), was successfully synthesized with excellent water stability and fluorescence properties. Due to the propeller structure of NTB ligands, a special topological structure of Co-MOF was shown: {2 4 .4 16 .6 8 }{2}4. It was proved that Co-MOF has great stability by soaking in different solvents for two weeks. Remarkably, the fluorescence quenching experiment verified that Co-MOF has excellent fluorescence sensor performance. Trinitrophenol, 2,4-dinitrophenol, and 2-amino-4-nitrotoluene (10 −5 M) with LOD of 9.00 × 10 −5 , 5.40 × 10 −5 and 5.07 × 10 −6 M can be detected via the process of fluorescence enhancement and quenching. Throughout the investigation, the mechanics of fluorescence quenching was performed. Due to the excellent UV absorption capacity of Co-MOF, it was a promising application to combine low-dimensional nanomaterials with sustainable biomass materials. A hybrid films of Co-MOF and cellulose acetate (CA) was generated. The hybrid films had highly transparency in the visible wavelength range and excellent UV-shielding ability owing to the CA/Co-MOF hybrid films enhanced the UV absorption capacity of Co-MOF.
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ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 16
·2110030
·
IF 19.924
Jun He,Hongli Liu,Fei Zhang,Xianggao Li,Shirong Wang
Poor crystallinity of perovskite and extensive defects around grain boundaries are the acknowledged hindrances to obtaining high efficiency and long-term stability for organic metal halide perovskite solar cells (PSCs). Here, a 2D covalent organic framework (2D COF) nanosheets, [(TPA) 1 (TPhT) 1 ] CN , is first in situ synthesized in a PbI 2 layer with a highly crystalline structure to precisely regulate the crystallization process of perovskite in the sequential deposition method. The existence of 2D COF nanosheets can decelerate intermolecular interdiffusion and induce perovskite crystals to grow along (110) planes with enlarged grain size. Meanwhile, 2D COF nanosheets distributed around the grain boundaries reduce the defect density and promote carriers transporting in the perovskite film. The superior properties of the perovskite film afford the champion PSC device with a power conversion efficiency of 22.04%, which is over 10% higher than the control device. Moreover, the target PSC also demonstrates outstanding long-term stability. It can maintain over 90% of its initial value after 90 days storage in ambient conditions for unencapsulated devices. This work paves a new path for regulating the crystallization process of perovskites via 2D crystalline materials.
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Catalysts
·
2022
·Vol. 12
·期 1
·62
·
IF 4.501
Xu Liao,Baoyou Pei,Ruixun Ma,Lingzheng Kong,Xilin Gao,Jiao He,Xiaoyan Luo,Jinqing Lin
The effective conversion of carbon dioxide (CO2) into cyclic carbonates requires porous materials with high ionic content and large specific surface area. Herein, we developed a new systematic post-synthetic modification strategy for synthesizing imidazolium-based hypercrosslinked ionic polymers (HIPs) with high ionic content (up to 2.1 mmol g−1) and large specific surface area (385 m2g−1) from porous hypercrosslinked polymers (HCPs) through addition reaction and quaternization. The obtained HIPs were efficient in CO2capture and conversion. Under the synergistic effect of high ionic content, large specific surface area, and plentiful micro/mesoporosity, the metal-free catalyst [HCP-CH2-Im][Cl]-1 exhibited quantitative selectivities, high catalytic yields, and good substrate compatibility for the conversion of CO2into cyclic carbonates at atmospheric pressure (0.1 MPa) in a shorter reaction time in the absence of cocatalysts, solvents, and additives. High catalytic yields (styrene oxide, 120 °C, 8 h, 94% yield; 100 °C, 20 h, 93% yield) can be achieved by appropriately extending the reaction times at low temperature, and the reaction times are shorter than other porous materials under the same conditions. This work provides a new strategy for synthesizing an efficient metal-free heterogeneous catalyst with high ionic content and a large specific surface area from HCPs for the conversion of CO2into cyclic carbonates. It also demonstrates that the ionic content and specific surface area must be coordinated to obtain high catalytic activity for CO2cycloaddition reaction.Keywords:hypercrosslinked ionic polymers;high ionic content;CO2cycloaddition;cyclic carbonates
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Yafei Sang,Zhe Shu,You Wang,Lizhi Wang,Du Zhang,Qin Xiao,Fa Zhou,Jianhan Huang
A series of bifunctional ionic hyper-cross-linked polymers were synthesized by the Friedel-Crafts reaction and ionic post-functionalization. The as-prepared polymers had high Brunauer-Emmett-Teller surface areas ( S BET , 623–1345 m 2 /g), considerable bifunctional ionic groups, namely bromide anions, and carboxyl groups. The polymer namely DHI-CSU-3-Br had a good CO 2 capture capacity (134 mg/g, 273 K, and 1.0 bar), moderate isotopic adsorption heat (28–38 kJ/mol), and excellent CO 2 cycloaddition ability. The catalytic experiments showed that 99% of propylene oxide was successfully converted to cyclic carbonate (70 °C, 0.1 MPa CO 2 , and 4 h). The catalytic activity of the polymer was easy to be recovered and it was repeatedly reused 5 times without significant reduction. This synthetic strategy for the preparation of the bifunctional ionic hyper-cross-linked polymers provided an alternative approach for CO 2 capture and catalytic conversion.
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2022
·
IF 3.898
Yuxin Wu,Zhuo Chen,Xiaohui Zhang,Jian Chen,Yundong Wang,Jianhong Xu
Carbon dioxide (CO 2 ) utilization and fixation have become one of the most important research areas nowadays due to the increase of global greenhouse effect. Cyclic carbonate, which is widely used in various fields, can be synthesized by fixation of CO 2 with epoxide in industry. Moreover, the synthesis of cyclic carbonate is a 100% atom economical reaction, which makes it eco-friendly and promising. To enhance the reaction efficiency and safety, a microreaction system was used as the platform for cycloaddition reaction. In this work, tetrabutylammonium bromide (TBAB) was chosen as catalyst, and propylene oxide (PO) as a mode substrate. Interestingly, the addition of water can increase the propylene carbonate (PC) yield and decrease the activation energy considerably, proving water as catalyst promoter for PC synthesis. PC yield and selectivity could reach 91.6% and 99.8%, respectively. The Influence factors and kinetic equation for CO 2 cycloaddition were obtained as well.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shuyue Li,Dongxu Yu,Lina Liu,Shiyu Yao,Xiaoqi Wang,Xu Jin,Dong Zhang,Fei Du
Rechargeable aqueous zinc-ion batteries (AZIBs) have attracted widespread attention as a sustainable energy storage system owing to the safe aqueous electrolyte. Manganese-based materials are potential cathodes for AZIBs, whereas, the dissolution of manganese would result in the significantly decline of capacity and unsatisfied lives. Herein, an in-situ electrochemical induced artificial solid electrolyte interphase (SEI), (Zn(OH) 2 ) 3 (ZnSO 4 )(H 2 O) 5 nanoflakes, is discovered to generate and coat on the surface of MnO@C in the initial charging process which could prevent the direct contact between the electrolyte and electrode with the result of inhibiting the excessive dissolution of manganese oxides. Benefiting from the artificial SEI, MnO@C exhibits an extremely excellent cycle performance with 0.003% capacity decay per cycle over 10,000 cycles without Mn 2+ additive in electrolyte. Moreover, MnO@C is proved to demonstrate a (de)intercalation reaction mechanism after the electrochemical activation process in initial charging process. The strategy proposed in this study provides a new proposal to develop high stable manganes oxide cathodes for AZIBs.
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