ACS Applied Materials & Interfaces
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2026
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IF 8.2
Zhixuan Ma,Pengxuan Wu,Bingshuang Li,Suhua Mao,Qian Liu,Hailun Xia,Jin Li,Zhen Xu,Xiaoxi Huang
The growing demand for green synthesis of hydrogen peroxide (H2O2) has fueled great interest in electrochemical synthesis via the oxygen reduction reaction (ORR). Carbon-based materials are an appealing class of electrocatalysts, offering the promise of tunable defects, heteroatom dopants, and controllable pore structures. However, increasing the accessibility of mesopores in carbon-based materials is challenging due to the restricted diffusion depth. In this study, we report the synthesis of a mesoporous carbon hollow shell with a big surface opening (C-750) and the nonhollow control material (C-750C). The hollow structure with a big surface opening facilitates rapid diffusion and transport of reactants and products through both its exterior and interior surfaces. This structure enables prompt reactant access to active sites and efficient product desorption, thereby yielding exceptional electrocatalytic ORR performance. In contrast, nonhollow mesoporous carbon materials rely solely on external surface diffusion, resulting in longer transport pathways, restricted accessibility to active sites, and product accumulation that diminishes reaction efficiency. In the rotating ring-disk electrode, C-750 demonstrates a higher diffusion-limited current density and higher H2O2 selectivity than C-750C, highlighting its superior mass transport efficiency due to the hollow structure as well as the large opening on the shell. In the flow cell, C-750 shows an industrial-level current density of ∼ −244 mA cm–2 at 0.28 V vs RHE, and the production rate of H2O2 is over 14.6 mol h–1 gcat–1. The density of edge defects, tailored by changing the carbonization temperature, works synergistically with oxygen dopants to enhance the catalytic performance, as confirmed by both theoretical simulations and experimental results.
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Polymers
·
2026
·Vol. 18
·期 1
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IF 4.9
Feihua Ye,Fan Chen,Yunhong Zhang,Yunwei Huang,Shasha Liu,Jiangfei Cao,Yanni Wu
Uric acid (UA), a key end-product of human purine metabolism, serves as an important biomarker linked to multiple disorders. This study developed a novel enzyme-free colorimetric sensing platform based on starch-derived nitrogen-doped biochar (NC) for the highly sensitive and selective detection of UA in human body fluids. The NC material with a high specific surface area and abundant nitrogen active sites was prepared via a two-step strategy involving hydrothermal synthesis followed by high-temperature pyrolysis, using starch and urea as raw materials. Under mild conditions, the NC effectively catalyzes dissolved oxygen to produce reactive oxygen species (·O2−and1O2), which oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) to a blue-colored oxidation product (TMBox). The presence of UA reduces TMBox to colorless TMB, leading to a measurable decrease in absorbance at 652 nm and enabling quantitative UA detection. Key reaction conditions were systematically optimized. Material characterization and mechanistic investigations confirmed the catalytic performance of the NC. The method demonstrated a wide linear response from 10 to 500 μmol·L−1, with a detection limit of 4.87 μmol·L−1, and demonstrated outstanding selectivity, stability, and reproducibility. Practical application in human serum and urine samples yielded results consistent with clinical reference ranges, and spike-recovery rates ranged from 95.5% to 103.6%, indicating great potential for real-sample analysis.
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ENVIRONMENTAL RESEARCH
·
2026
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IF 7.7
Hongliang Chen,Nana Lu,Qian Long,Mengbi Yang,Dandan Luo,Zhipeng Wang
A porous composite catalyst, designated as 0.1Co/RM@G, is successfully fabricated with red mud (RM). This catalyst, incorporating CoFe 2 O 4 , Fe 3 O 4 and Na 4 CoO 3 as active species, is employed to activate peroxymonosulfate (PMS) for the methylene blue (MB) degradation in aqueous solutions. The results demonstrate that under optimal conditions: 1 g/L of 0.1Co/RM@G and 10 mM PMS, the removal efficiency of MB (initial concentration: 100 mg/L) achieves up to 99.7 % within 15 min. Radical scavenging experiments combined with electron paramagnetic resonance (EPR) analyses confirm that singlet oxygen ( 1 O 2 ) is the primary reactive oxygen species (ROS) responsible for the MB degradation. A plausible mechanism for PMS activation by 0.1Co/RM@G is proposed, where the synergistic effect between Co 3+ /Co 2+ and Fe 3+ /Fe 2+ redox cycles plays a crucial role in sustaining the high catalytic performance. Furthermore, recycling experiments reveal that the catalyst retains over a 71.3% MB removal efficiency after four cycles, highlighting its strong reusability. Density functional theory (DFT) calculations suggest that the N sites (30, 21) and C sites (13, 6, 15, 11, 2, 4) on the MB molecule are particularly susceptible to attack by 1 O 2 during the oxidation process. The potential pathways for the MB degradation are proposed through intermediates analysis using LC-MS technology. Thanks to its robust catalytic efficiency and excellent recyclability, the 0.1Co/RM@G composite shows a great potential for practical applications in the treatment of MB wastewater.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 21.1
Qi Zhou,Jiale Wang,Jiaojiao Song,Hao Yan,Ruiyan Wang,Tiantian Luo
A mesoporous N-doped carbon bearing atomically dispersed Fe (Fe 1 -N-Cv) was created that uniquely couples carbon-vacancy and pore engineering to switch the electron spin state of highly accessible Fe sites from low-spin (t 2 g 5 e g 0 ) to high-spin (t 2g 3 e g 2 ), thereby unlocking superior Fenton-like activity. The material was synthesized by pyrolyzing Fe-encapsulated ZIFs under negative pressure, whereby the built-in pressure gradient simultaneously enlarged pores and generated carbon vacancies. Fe 1 -N-Cv degrades pollutants 3.89-fold faster than conventional Fe 1 -N-C, maintains > 99 % tetracycline removal and > 95 % mineralization during 240 min of continuous flow operation, operates over a pH range of 3.0–9.0, and shows stable recyclability and strong resistance to coexisting matrix constituents. Mechanistic analysis identifies a non-radical regime dominated by singlet oxygen, assisted by high-valent Fe-oxo and electron-transfer pathways, while DFT calculations show that carbon defects accelerate interfacial charge transfer and lower the free-energy barrier for PMS activation. Synergistic engineering of carbon vacancies and pores thus emerges as a powerful lever to modulate both the geometric accessibility and electronic spin state of single-atom Fe centers, directly translating into markedly enhanced Fenton-like performance. This strategy offers a promising approach for boosting single-atom-catalyst activity and robustness, advancing their practical deployment in continuous environmental remediation technologies.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.7
Danhua Jiao,Ying Li,Runjie Wang,Tianxue Li,Xiaodong Cai,Qizhao Wang
The Photo-Fenton-like reaction offers a novel avenue for the efficient and thorough mineralization of emerging pollutants while is constrained by metal ion leaching and a declination in catalytic performance. This study presented the development of a ZnFe 2 O 4 /NBGA (named as ZFO/NBGA) catalytic system including strategically established Fe-X-C (X = N, B) links and a three-dimensional hierarchical architecture. The Fe-X-C bond functions as a conduit to modulate the charge environment at active sites, and the three-dimensional nitrogen and boron-doped graphene aerogel (noted as NBGA) accelerates charge and ion transfer. Experimental findings demonstrated that the ZFO/NBGA catalytic system achieved 99.5% TC removal activity for PDS activation under visible light irradiation within 50 min. The reaction rate constant (k) reached 9.9 × 10 −2 min −1 , which is 6.6 times higher than that of pure ZnFe 2 O 4 . Additionally, the anti-interference ability in complex water environments was validated. Crucially, the catalyst exhibited exceptional stability and economic sustainability, maintaining 79.89% degradation efficiency after 6 consecutive cycles with negligible metal leaching (Zn < 1.0 mg/L, Fe < 0.3 mg/L). The primary active species were • O 2 − , h + , and 1 O 2 . LSCM evaluated the degradation pathways of contaminants, and the toxicity of the resultant chemicals were examined. DFT calculations elucidated that improved performance resulted from directional electron transport, which prolonged carriers life-time, and the d -band center of ZFO/NBGA, situated closer to the Fermi level, optimized the adsorption and desorption of intermediates. This work may offer novel insights into the mechanisms of metal-based carbon catalysts for the efficient remediation of emerging pollutants, which is essential for the establishment of ecologically sustainable catalytic approaches.
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Journal of Water Process Engineering
·
2026
·
IF 6.7
Xiao Liu,Runze He,Jiachen Song,Xinyu Hou,Fei Wang
With the growing severity of environmental pollution, the treatment of organic wastewater and waste plastic bottles has become global concerns. This study explored the feasibility of synthesizing metal-organic composite catalysts using waste PET plastic by a microwave one-step synthesis process with only 4 h. Comprehensive characterizations confirmed that the bimetallic Cu/Mn-PET catalyst outperformed monometallic counterparts and pure BDC-derived catalysts, featuring a more regular polyhedral morphology, good crystallinity and excellent stability. XPS valence state analysis uncovered pronounced synergistic interactions between Cu and Mn. Notably, despite a relatively low specific surface area (11.75 m 2 /g), Cu/Mn-PET featured the highest active site density and exhibited minimal interfacial charge transfer resistance in electrochemical measurements. When combined with PMS-AOPs technology, Cu/Mn-PET achieved nearly 100% degradation efficiency for various pollutants (dyes, antibiotics, phenolic compounds) under optimized conditions, accompanied by substantial mineralization (TOC removal rates above 56.36%). Additionally, the Cu/Mn-PET catalyst also showed strong recyclability with low metal leaching concentrations, as well as good salt tolerance. Furthermore, it was proved that the catalytic mechanism of Cu/Mn-PET involved the combined action of free radical reactions and non-free radical reactions, but the non-free radical based 1 O 2 played a dominant role. Thus, a green and efficient PET microwave one-step conversion technology has been developed to prepare a bimetallic organic composite catalyst with high catalytic activity and stability successfully, which hold significant implications for environmental protection and resource utilization.
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ACS Applied Nano Materials
·
2026
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IF 5.5
Zhiyun Xu,Mengyuan Zhang,Wentao Zhang,Dandan Han,Yongsheng Zhang,Tianliang Lu,Renfeng Nie,Xiaoqin Si,Chunbao Xu,Dan Wu,Jianshe Wang
The regulation of metal-acid bifunctional sites is of great significance in heterogeneous catalysis. In this study, commercial Pt/Al2O3 catalysts were modified by ethyl iodide under reductive conditions to prepare I–Pt/Al2O3 catalysts with intimate metal-acid bifunctional sites for the selective hydrogenolysis of furfuryl alcohol to 1,2-pentanediol. Electron transfer from Pt nanoparticles to I results in the formation of a negatively charged I adatom on the positively charged Pt surface, which induces on-surface hydrogen spillover to form Pt(H–)–I(H+) metal-acid bifunctional sites under a hydrogen atmosphere. By modulating the I coverage, the ratio between metal and acid sites on the catalyst surface can be finely adjusted at the nanoscale, providing a tunable hydrogenolysis selectivity of th furan ring toward 1,2- or 1,5-pentanediol. The selectivity for 1,2-pentanediol was promoted from 17.2% over the initial Pt/Al2O3 catalyst to 67.0% over I–Pt/Al2O3 catalysts at full furfuryl alcohol conversion. The developed Pt–I catalyst with controllable metal-acid bifunctional sites holds great promise for the catalytic upgrading of biomass-derived molecules.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 21.1
Meng Li,Liyao Zeng,Peitong Cen,Ziyin Xia,Jiaqian Zhang,Lei Huang,Jia Yan,Shaoqi Zhou,Ce-Hui Mo,Xiangkang Zeng,Hongguo Zhang
This work introduces an innovative stacked iron mesh electrode configuration to achieve accelerated degradation of perfluorooctanoic acid (PFOA) by synergistically coupling electrochemical oxidation with peroxymonosulfate (PMS) activation. The system was systematically evaluated through electrochemical measurements, free radical quenching, and electron paramagnetic resonance spectroscopy, complemented by density functional theory calculations. The optimized triple-layer Fe electrode demonstrated outstanding performance, attaining nearly complete PFOA removal (100 %) within 12 min and a high kinetic rate constant of 0.218 min –1 . DFT analysis revealed that the Fe mesh possessed the strongest PMS adsorption energy (–2.68 eV) and the shortest Fe–O bond length (2.24 Å), confirming its superior activation capability. Mechanistic studies confirm the effectiveness of the electron transfer coupled with the hydroxyl radicals in defluorination and decarbonization during PFOA degradation. In addition, the system exhibited high cycle stability and strong tolerance to various background ion under continuous operations in the amplification experiment. The system also exhibited superior performance and low leaching of metal ions in treating various organic pollutants of practical wastewater (fluoride wastewater and landfill leachate). These findings present an effective and practical strategy for the remediation of persistent per- and polyfluoroalkyl substances in contaminated water sources.
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Processes
·
2026
·Vol. 14
·期 2
·223
·
IF 2.8
Tianran Kong,Annan Zhao,Yinghui Zhang,Zongxuan Bai,Hongying Lü,Kaixuan Yang
Efficient conversion of biomass-based platform molecules into high-value derivatives is recognized as one formidable challenge in biomass upgrading. In this work, a one-pot deep eutectic solvents-assisted solvothermal method was developed for the modification of the commercial Pt/C catalysts by introducing a secondary metal (M = Sn, Bi, Ge, Sb, Pb). The structural and electronic properties of the catalysts were precisely tuned. Among the screened metals, the addition of Sn yielded the most significant improvement in catalytic activity. The optimized PtSn0.5/C-140 catalyst achieved superior furfural (FAL) conversion and furfuryl alcohol (FOL) selectivity under mild conditions (20 °C, 2 MPa H2). Comprehensive characterizations, including XRD, HRTEM, XPS, and H2-TPD, confirmed the formation of Pt-Sn solid-solution phase. Furthermore, Characterization and reaction results revealed that the electronic and geometric effects induced by Sn modulated Pt active sites, significantly enhancing the adsorption of the active H species. Additionally, the SnOxspecies adjacent to the Pt-Sn sites served as hydrogen spillover acceptors, further accelerating the hydrogenation process. The synergy between the Pt-Sn solid-solution phase and SnOxspecies is identified as the origin of the superior performance at room temperature. These findings provide a new strategy for the design of high-performance biomass conversion catalysts by upgrading commercial noble metal catalysts.
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Nature Communications
·
2026
·
IF 15.7
Zhang Xinyi,Wang Liangjie,Wei Jian,Guo Zhuang,Liu Xinyao,Duan Lijie,Zhao Huazhang,Song Yonghui
Oxygen vacancies (O v ) on metal oxide surfaces exhibit high catalytic activity for activating peroxymonosulfate (PMS) in wastewater decontamination, yet their in-situ regeneration remains a significant challenge. This study successfully achieves in-situ real-time regeneration of O v on CuO surfaces through simple alkali etching without interrupting the contaminant removal process. The surface hydroxyl groups introduced by alkali treatment significantly reduce the formation energy of O v on CuO surfaces from 1.60 eV to 0.38 eV. Both experimental results and density functional theory calculations reveal that the high activity of CuO relies on the synergy of surface hydroxyl groups and O v . This synergy increases the antibonding states below the Fermi level and the electron spin density of Cu near O v , thereby promoting electron transfer from CuO to PMS. As a result, by just adding an equimolar amount of alkali relative to PMS in CuO/PMS system, the degradation rate constant of sulfamethoxazole (SMX) greatly increases by 42 times. The primary reactive oxygen species in this system are sulfate radicals and hydroxyl radicals. Furthermore, OH - /CuO/PMS system exhibits a long-term stability (> 300 h) for SMX removal in a real water matrix. This work provides a highly executable method to in-situ real-time regenerate O v on CuO surfaces, representing significant progress in the critical yet underappreciated field of catalyst regeneration.
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Journal of Water Process Engineering
·
2026
·
IF 6.7
Tianyuan Xu,Nanxi Zhu,Ruina Yuan,Yaowen Xing,Xiahui Gui
Carbon-driven persulfate (PS) activation is promising for antibiotic degradation, but conventional carbon catalysts often require thermal/acid-base modification or metal doping, suffering from low yields and high costs. Herein, we innovatively employed unmodified low-rank coals from Shengdong (LC SD ) and Sujiagou (LC SJG ) as cost-effective PS activators for sulfamethazine (SMZ) degradation. Characterizations including Raman, 13 C nuclear magnetic resonance, and electron paramagnetic resonance (EPR) revealed distinct structural-chemical features. LC SJG had more structural defects, –OH, and –COOH groups, while LC SD showed higher persistent free radical and C O group concentrations. LC SJG exhibited superior performance (99.3 % SMZ removal in 120 min) versus LC SD (84.2 %) and good tolerance to coexisting ions, indicating practical application potential. Possible degradation pathways of SMZ, as revealed by high-performance liquid chromatography-mass spectrometry, were proposed involving sulfonamide cleavage and pyrimidine ring opening. Mechanistic investigations via EPR, radical quenching, and electrochemical analysis revealed that 1 O 2 dominated SMZ degradation (59.3 %) in the LC SD /PS system via C O groups. Conversely, • OH and SO 4 •− contributed 62.7 % to degradation in the LC SJG /PS system through structural defects and –COOH groups. Overall, this study provides a novel strategy for developing low-cost, high-performance PS activators tailored for wastewater treatment.
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Desalination and Water Treatment
·
2026
·
IF 1
Yuqiong Gao,Qingqing Yang,Jiaxin Ma,Juxiang Chen,Cong Li,Naiyun Gao
This study employs the Fe(III)/CaSO 3 system to degrade ibuprofen (IBP) and elucidate the key factors and mechanisms. Negligible IBP degradation is observed when CaSO 3 and Fe(III) are applied individually, but their combination significantly enhances it. At initial pH 3, 40 μΜ Fe(III), and 200 μM sulfite, 92.2 % of IBP was removed within 20 min. Quenching experiments indicated that SO 4 •– , •OH, and 1 O 2 collectively governed the degradation of IBP in the Fe(III)/CaSO 3 system. Additionally, dissolved oxygen is essential in the system by initiating the radical chain reactions. The degradation of IBP by the Fe(III)/CaSO 3 system is influenced by key operational parameters and the water matrix. Typically, the process exhibits optimal Fe(III) and sulfite concentrations and initial pH, an activation energy of 51.2 kJ·mol -1 , and is inhibited by common water constituents like humic acid (HA), Cl⁻, Br⁻ and Mg 2+ . Integrated LC/TOF/MS and DFT calculations identified hydroxylation and decarboxylation as the primary pathways for IBP degradation, with bioassays confirming decreased antibacterial activity due to toxic products. Overall, our finding indicate that the Fe(III)/CaSO 3 system is effective for the oxidation of IBP, but the process parameters need further optimization to enhance IBP degradation efficiency and reduce potential environmental risks.
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