ACS ES&T Engineering
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2026
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IF 6.3
Xu Pan,Jiangkun Xie,Mingze Jiao,Liang Shan,Hongyuan Qi,Wenjun Huang,Zan Qu,Naiqiang Yan,Haomiao Xu
Methane selective catalytic reduction (CH4-SCR) represents a promising strategy for nitrogen oxides (NOx) abatement, yet its practical application is hindered by catalyst deactivation in the presence of water, caused by competitive adsorption on acid sites and irreversible hydroxylation of active metal species. In this study, we developed a dual-functional In@H-Beta/Fe2O3 catalyst through sequential ion-exchange and impregnation. This architecture confines indium species within the channels of H-Beta zeolite, while Fe2O3 nanoparticles are dispersed on the external surface, creating a synergistic system featuring a hydrophobic layer and strong Fe–O–In interfacial interactions. Under 5% H2O conditions, the optimized catalyst achieves 85% NOx conversion (vs 40% for conventional In@H-Beta). The enhanced water resistance is attributed to two factors: first, Fe2O3 establishes a physical barrier that protects acid sites and stabilizes InO+ active sites via Fe–O–In bonding, thereby inhibiting hydroxylation; second, strong interfacial Fe–O–In interactions further stabilize InO+ active sites against aqueous deactivation. Additionally, the Fe2+/Fe3+ redox cycle is proposed to facilitate O2 activation. In situ DRIFTS studies under 5% H2O confirm effective CH4 activation, as indicated by markedly more intense C–H stretching bands compared with In@H-Beta. The reaction pathway involves NO activation over Brønsted acid sites to form nitrate species, and CH4 activation on InO+ sites generating methyl radicals, which subsequently participate in NOx reduction. This work offers a new design strategy for developing highly active and water-tolerant CH4-SCR catalysts suitable for industrial flue gas treatment.
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ACS Catalysis
·
2026
·
IF 13.6
Jun-Bin He,Lian Wu,Wenli Yuan,Hai-Xue Pan,Binju Wang,Gong-Li Tang
Achieving highly regioselective C–H bond functionalization at the bridgehead carbon of a single molecule is a fascinating, yet formidable challenge. BcmD, a P450 enzyme, catalyzes the regioselective hydroxylation at the sp3-hybridized bridgehead carbon of the bicyclo[4.2.2]piperazinedione ring scaffold during bicyclomycin biosynthesis. Herein, we provide mechanistic details of BcmD to understand its substrate binding and the origin of its regioselectivity. The high-resolution structure of SoBcmD from Streptomyces ossamyceticus in complex with its natural substrate, together with site-directed mutagenesis and computational simulations, reveals that the precise substrate positioning, enabled by specific hydrogen-bonding and hydrophobic interactions with crucial residues, determines the regioselectivity. Intriguingly, we identify SoBcmD as a peroxygenase that could utilize H2O2 as an oxidant to catalyze regioselective hydroxylation. Mechanistic analysis indicates that H2O2 activation in SoBcmD involves a homolytic cleavage process, mediated by a hydrogen-bonding network comprising residues T277, A273, and the substrate. Furthermore, structure-based channel analysis and mutagenesis demonstrate that the I157V mutant exhibits significantly enhanced peroxygenase activity. These findings advance our understanding of regioselectivity control in BcmD and provide valuable guidance for engineering P450 peroxygenases for the C–H bond activation at the chemically challenging bridgehead carbon sites.
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JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2026
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IF 4.4
Haoyi Xu,Xiaoning Deng,Ying Zhang,Yuwei Pan
Chelating agents significantly enhanced SDZ degradation in UV/Fe 2+ /H₂O₂ system. • The CA-enhanced systems operate efficiently across pH 3–8. • OH was the dominant reactive species, O₂· − and 1 O₂ played minor roles in SDZ removal. • Degradation pathways produced intermediates with lower toxicity than SDZ. • The system showed broad-spectrum reactivity and stability in natural freshwater. Antibiotics, widely detected in aquatic environments, pose significant threats to ecosystems and human health due to their recalcitrance in conventional wastewater treatment processes. This study systematically investigated the enhancement effects and mechanisms of three chelating agents (CAs) including NTA, EDTA and EDDS on sulfadiazine (SDZ) degradation in the UV/Fe 2+ /H₂O₂ system. Results showed that CAs significantly improved SDZ removal efficiency by complexing iron ions, promoting Fe 2+ /Fe 3+ cycling thereby enhancing photo-induced Fenton reactions. The NTA/UV/Fe 2+ /H₂O₂ system exhibited the highest performance, achieving 90.5% SDZ removal within 20 min, followed by EDTA (90.1%) and EDDS (88.7%) and without CAs (<35%). The CAs/UV/Fe 2+ /H₂O₂ system maintained high efficiency over a broad pH range (3–8), overcoming the pH limitation of traditional UV-Fenton processes. Electron paramagnetic resonance (EPR) and quenching experiments confirmed ·OH was the dominant reactive oxygen species and O₂· − and 1 O₂ also played minor roles. Degradation pathways of SDZ included ·OH oxidation, S N bond cleavage, and ring-opening reactions, producing intermediates with lower toxicity than SDZ. Meanwhile, the CAs/UV/Fe 2+ /H₂O₂ system could effectively remove various antibiotics (e.g., sulfamethoxazole, tetracycline) and maintain stability in the presence of inorganic anions and humic acid. Moreover, the CAs/UV/Fe 2+ /H₂O₂ system performed well in natural fresh water matrices, highlighting its practical application potential for antibiotic-contaminated water treatment. Download: Download high-res image (100KB) Download: Download full-size image
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JOURNAL OF ORGANIC CHEMISTRY
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2025
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IF 3.6
Qiujie Shan,Lu-Lu Chai,David James Young,Zhi-Gang Ren,Hong-Xi Li
The light-promoted, nickel-catalyzed hydrogen-evolution C(sp3)–H acylation of simple alkanes with aromatic aldehydes has been achieved without the need for additional photosensitizers or oxidants. This reliable and atom-economical reaction afforded a broad range of aryl alkyl ketones in good yields, with H2 as the sole byproduct. It was successfully demonstrated on a gram scale as well as for the postfunctionalization of drug molecules. Aromatic aldehydes play multiple roles, including a photosensitizer, a coupling partner, and a hydrogen atom transfer agent.
研究领域:
有机化学
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催化化学
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光化学
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绿色化学
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药物化学
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合成化学
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高影响因子
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
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2023
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IF 5.7
Yage Li,Shuaibing Wu,Feng Liang,Gongye Lv,Yu Tian,Haijun Zhang,Yong Liu,Guoqi Liu
Rod-like h-BN with an average diameter of 2 µm was synthesized at a relatively low temperature of 1200 °C through a catalytic pyrolysis precursor strategy using boric acid and melamine as starting materials, and Co(SO 3 NH 2 ) 2 ·4 H 2 O as a catalyst precursor. Subsequently, novel low-carbon Al 2 O 3 -C refractories were prepared via a replacement of the graphite with the as-synthesized rod-like h-BN. When 1 wt% h-BN rods were added to replace graphite, after 3 h coking at 1400 °C, the cold modulus of rupture, cold compressive strength , oxidation resistance , and thermal shock resistance of the specimen were increased by 16.4%, 24.8%, 31.2%, and 52.2%, respectively, compared with these of the control specimen. Moreover, the introduction of h-BN rods in the matrix enhanced the non-wetting ability of the refractory with molten slag, thus the rod-like h-BN modified low carbon refractory presented better slag corrosion resistance with reference to the specimen without h-BN rods.
研究领域:
材料科学
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耐火材料
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高温性能
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2026
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IF 6.2
Kuan Gao,Qin Geng,Wenhui Zhang,Xin Li,Ping Tong,Anshu Yang,Zhihua Wu,Hongbing Chen
The effects of pH-shifting combined with quercetin binding on peanut Ara h 2 were evaluated using multispectroscopy, cell models, molecular simulation, and correlation analysis. After dual treatment, Ara h 2 exhibited significant structural changes, as evidenced by decreased intrinsic fluorescence and converted α-helix into β-sheet, leading to reduced IgE-binding capacity and diminished ability of dendritic cells and T cells to differentiate toward the Th2 pathway due to the masking of epitopes. Moreover, the binding sites of quercetin gradually shifted toward the hydrophobic core of Ara h 2 with pH changes, which inhibited fluctuations in the aa50–70 region. Finally, according to the correlation analysis, pH-shifting combined with quercetin binding may reduce the allergenicity of Ara h 2 by the migration of many Trp and Tyr residues to the protein surface, which disrupted the conformational epitopes. Therefore, this study provides an approach for the development of hypoallergenic peanut products.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2026
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IF 4.7
Baomin Wang,Haoxiang Yang,Chengcheng Fan,Fei Liu,Wenxin Lu
Alkali-activated materials show excellent capture capacity on heavy metals, but the mechanisms to immobilize heavy metals remain inadequately explored. This work investigated the main hydration product C-A-S-H gels for encapsulation of heavy metals such as Pb(II), Zn(II) and Cd(II). Furthermore, the adsorption behavior and mechanisms of Pb(II) in pore solutions by C-A-S-H were examined. These findings reveal that aluminum is incorporated into the silicon chains of C-S-H in the form of aluminum-oxygen tetrahedra, thereby generating C-A-S-H. The bonding ratio, which depends on the Ca/Si ratio, reaches its peak value of 0.139 when the Ca/Si ratio is 0.9. In highly alkaline environments, amphoteric Pb(II) and Zn(II) form hydroxyl coordination polyhedra, enhancing silicon chain polymerization, whereas Cd(II) is immobilized via ion exchange with Ca(II), resulting in solid solutions. For C-A-S-H with a Ca/Si ratio of 0.6, Pb(II) adsorption occurs predominantly through physical interactions. However, as the Ca/Si molar ratio increases, the effect chemisorption and ion exchange become more significant along with the formation of Pb 8 Ca(Si 2 O 7 ) 3 . C-A-S-H gel with a Ca/Si ratio of 0.9 has the highest Pb(II) adsorption capacity, reaching 92.55 mg/g.
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ACS Applied Materials & Interfaces
·
2026
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IF 8.2
Yuan Ma,Yongli Li,Lan Jiang,Xin Kong,Xin You,Liang Liu,Rui Bao,Zhenhua Ge,Hao Cui,Feng Liu,Jianhong Yi
The energy-intensive Haber-Bosch process for ammonia synthesis necessitates sustainable alternatives, electrochemical nitrate reduction (eNO3RR) is emerging as a promising route to address nitrate pollution. However, it faces a critical bottleneck: the low ammonia selectivity arising from competitive hydrogen evolution. Herein, we introduce copper carbon dots-supported iron phthalocyanine (Cu-CDs/FePc) - a electrocatalyst featuring dynamic Cu–Fe dual sites that steer tandem e–/H+ delivery for efficient NH3 electrosynthesis. It achieves an outstanding ammonia yield of 17.69 mg h–1 mgcat.–1 with a remarkable Faradaic efficiency of 91.0% at −0.7 V vs RHE in acid conditions, which surpasses many reported transition metal-based electrocatalysts for eNO3RR. In-situ FTIR spectroscopy and density functional theory (DFT) calculations elucidate that dynamic Cu–Fe dual sites orchestrate directional electron–proton relay chains through electronic complementarity: Electron-deficient Cu2+ centers intensify NO3– adsorption/activation, while electron-enriched Fe2+ sites drive *NO2 protonation, and interfacial charge shuttling initiates valence oscillations (Cu+/Cu2+ and Fe2+/Fe3+) effectively lower rate-determining step energy barrier, thereby boosting ammonia selectively while simultaneously suppressing hydrogen evolution. Furthermore, the catalyst exhibits robust stability over 100 h and practical versatility in zinc-air battery systems. This work presents a rational design strategy for high-performance eNO3RR catalysts, offering a significant advance toward efficient green ammonia synthesis and environmental remediation.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Yanhua Lei,Mengchao Ding,Sha Cheng,Da Huo,Fei Zhang,Tao Liu,Yuliang Zhang
The transition metal sulfide MoS 2 has attracted great interest from the scientific community as an excellent co-catalyst for promoting Fe 2+ /Fe 3+ cycling in advanced oxidation processes to enhance the efficiency of H 2 O 2 decomposition. A photothermal-enhanced photo-Fenton pollutant degradation strategy was proposed. Hybrids of magnetically recyclable Fe 3 O 4 fabricated 1 T-2 H MoS 2 (1 T-2 H MoS 2 @Fe 3 O 4 ) with excellent photothermal conversion efficiency were fabricated to overcome the limitations of relatively low catalytic activity and cycling stability in Fenton reaction. XRD , Raman, TEM and hysteresis loop were employed to evaluate the heterogeneous phase 1 T-2 H MoS 2 nanoflowers as well as the magnetic property . The 1 T-2 H MoS 2 @Fe 3 O 4 hybrids with excellent photothermal conversion efficiency not only enhance the reaction temperature of the Fenton reaction occurring on the material surface, but also demonstrate an effective interfacial photothermal water evaporation efficiency. Due to the synergistic effect of photocatalysis and photo-Fenton catalytic reaction , a quick degradation of simulated pollution were achieved in 5 mins with 98.3% degradation, which could be further improved to 99% due to the photothermal promoting reaction. The 1 T-2 H MoS 2 @Fe 3 O 4 hybrids exhibit good magnetic recyclability, cyclic stability and photothermal performance, which endow it a wide potential application in the field of environmental remediation and the field of water evaporation at the photothermal interface, etc.
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CERAMICS INTERNATIONAL
·
2022
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IF 5.532
Zheng-Bai Zhao,Cheng Hu,Yang Wang,Hong-Min Cong,Yong Ma,Ding-Duo Lin,Wei-Li Li,Chao Yan
The solvent-based resins have been applied widely in the preparation of thermal interface material (TIM). However, the use of solvents is harmful to the environment and human health. To address this, an environment-friendly TIM is fabricated by employing waterborne epoxy as a polymer matrix in this research project. The waterborne epoxy resin/polyvinyl pyrrolidone/hexagonal boron nitride (WER/PVP/h-BN) composite is successfully prepared through a facile method. First, the WER/PVP/h-BN mixture is obtained by a one-pot process. Subsequently, the WER/PVP/h-BN composite is fabricated by heat curing. The thermal conductivity of obtained WER/PVP/h-BN composite can reach 1.0921 W/m·K at 40 wt% filler loading. The mechanism of PVP for thermal conductivity enhancement of composites is demonstrated utilizing effective medium theory (EMT) and Fogyel’s models. Furthermore, the mechanical, electrical, and surface properties of WER/PVP/h-BN composites are comprehensively investigated. The valuable information and insight for the design and preparation of environment-friendly TIMs are provided in this paper.
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ENERGY & FUELS
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2022
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IF 4.654
Xianqiang Huang,Yanan Cui,Gang Liu,Haitao Wang,Junyu Ren,Yalin Zhang,Guodong Shen,Lingling Lv,Huai-Wei Wang,Yi-Fa Chen
With the arising concern of environmental problems, the removal of polycyclic aromatic hydrocarbons or sulfides in fuel oils is an indispensable process to achieve a clean energy source. At present, direct catalytic oxidation of benzyl C–H bonds of polycyclic aromatic hydrocarbons and sulfides to corresponding carbonyl compounds is very attractive, yet their simultaneous oxidation using a single economical-friendly catalyst is not yet well established. Here, three imidazole-decorated copper polyoxomolybdate frameworks (Im-Cu-PMoFs) are successfully synthesized by tuning different imidazole derivatives. These Im-Cu-PMoFs can serve as effective heterogeneous catalysts for the one-pot oxidation of benzylic hydrocarbons and sulfides to produce carbonyl compounds. Specifically, Im-Cu-PMoFs-3 as a single component catalyst exhibits high activity and prominent selectivity (conversion up to 99% and selectivity up to 99%) in the one-pot reaction. In addition, the possible reaction pathway and active sites are supported by sufficient characterizations and DFT calculations, which reveal the synergistic effect of Mo(VI) and Cu(II) centers in the one-pot catalysis reaction. These dual function-validated frameworks hold much promise in the exploration of novel catalysts for applications like continuous catalytic or flow bed reaction.
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POLYMER COMPOSITES
·
2023
·Vol. 44
·期 10
·6440-6453
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IF 5.2
Bi Yang,Beibei Chen,Wenquan Dong,Yang Tong,Jiaye Li
Polymer self-lubricating composite coatings have been widely used on the surface of machinery to extend the life of the moving systems/parts by controlling friction and wear. In this work, epoxy nanocomposite coating with the thickness of about 60 μm was fabricated with addition of hexagonal boron nitride nanosheets (BNNSs)/CeO 2 nanohybrid for enhancement in antifriction and wear resistance. The active BNNSs were first obtained by exfoliating h-BN with alkaline solution, and then the rare earth oxide of CeO 2 nanoparticles were immobilized on the surface of BNNSs through hydrothermal method. The microstructure morphology and chemical composition of as-proposed BNNSs/CeO 2 were characterized by field emission scanning electron microscopy, HRTEM, Fourier transform infrared spectroscopy, RS, X-ray diffraction, and X-ray photoelectron spectroscopy. And the tribological behaviors of epoxy nanocomposite coatings containing BNNSs, CeO 2 , and BNNSs/CeO 2 were investigated comparatively using ball-on disc friction tester (MPX-3). And the 440C stainless-steel ball with diameter of 8 mm was used as the counterface material. Tribological tests showed that epoxy-BNNSs/CeO 2 had the best friction and wear reduction properties, and the lowest coefficient of friction and wear rate of epoxy-based composite coating were achieved when the content of BNNSs/CeO 2 was 0.5 wt%, with 84.9% and 96.3% reduction, respectively. Moreover, the effect of sliding conditions on the tribological performance of epoxy-BNNSs/CeO 2 was investigated. The corresponding enhancing mechanisms of BNNSs/CeO 2 were discussed as well.
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