COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
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IF 3.99
Qingwen Long,Feng Liu,Yanjie Yuan,Yuting Dai,Chunli Wang,Xuheng Li,Jing Zhang
In this study, heterogeneous Fenton-like catalyst, nano-Fe° encapsulated in hydrothermal carbon (Fe°/HTCC), was prepared via a green chemistry route, aiming at increasing the degradation efficiency of p-chlorophenol (4-CP) by controlling the stability of the catalyst and Fe(III)/Fe(II) cycling in the advanced oxidation process. The degradation of 4-CP by heterogeneous Fenton reactions was conducted with the assistance of visible light, which was monitored with the aid of the HPLC and total organic carbon analysis. The results revealed that Fe°/HTCC composite markedly enhanced both the degradation (100 %) and the mineralization efficiency (∼73.9 %) for 100 mg/L 4-CP within 60 min at pH 4.0. More importantly, the catalyst presented a high stability to resist the side oxidation, where the removal efficiency was maintained even after 5 successive cycling experiments. Electron spin resonance confirmed that in the presence of both HTCC and visible light irradiation greatly enhanced the production of •OH for the degradation and mineralization of 4-CP, which can be attributed to the enhancement of Fe(III)/Fe(II) cycling. This study paves a new way toward the rational design of Fe°–carbon composites as heterogeneous Fenton-like catalysts for potential applications into wastewater treatment.
研究领域:
环境科学
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
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2021
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IF 7.086
Bingzhi Liu,Tingyu Pan,Jiajun Liu,Li Feng,Yuning Chen,Huaili Zheng
Chlorophenol is a widely used organic compound, and the environmental and health problems caused by it have being worsened in recent years. This study used 2,4,6-trichlorophenol (2,4,6-TCP) as the target pollutant, and employed ultrasound (US) enhanced zero-valent iron (Fe 0 )/EDTA/air system (FEA), namely US/FEA, to remove 2,4,6-TCP. The influence of single factor experimental conditions such as EDTA concentration, Fe 0 dosage, US power, pH and pollutant concentration on the removal efficiency of 2,4,6-TCP was investigated, and the optimal reaction conditions were determined. The mechanism of reactive oxygen species (ROS) produced by US/FEA was explored. The degradation process and removal mechanism of 2,4,6-TCP in the US/FEA were discussed through the determination and analysis of intermediate products. The results showed that US could continuously activate and renew the Fe 0 surface, accelerate its oxidation and corrosion process, and then continuously and stably produce sufficient amounts of Fe 2+ and Fe 3+ . Ultrasonic cavitation effect could reduce the difficulty of O 2 activation reaction, and promote the production of sufficient H 2 O 2 . The addition of EDTA made the system have a wide range of pH applications, and its performance under neutral and alkaline conditions was also superior. The ROS of US/FEA included ·OH, O 2 ·- and Fe(IV), where Fe(IV) was the main contributor to the removal of 2,4,6-TCP. In addition, the degradation of 2,4,6-TCP had two processes including dechlorination and benzene ring opening. First, 2,4,6-TCP was dechlorinated and degraded into phenol. And then, phenol was degraded into small molecular acids by ring-opening, and finally it was mineralized into CO 2 and H 2 O completely. US/FEA is a promising technology for high-efficiency degradation of organic matter and deep environmental purification.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMOSPHERE
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2019
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IF 5.108
Kané Rabé,Lifen Liu,Noor Ahmed Nahyoon
Visible-light-driven photocatalytic Fuel Cell (PFC) is of great interest in the environmental pollutant remediation with energy recovering. Herein, enhancement in photocatalytic degradation of Tetracycline Hydrochloride (TC) with electricity generation was achieved in a single reactor of PFC with paired stainless-steel mesh electrode loaded with anodic g-C 3 N 4 /Fe 0 (1%)/TiO 2 and cathodic WO 3 catalyst (at various pH, 0.05 M Na 2 SO 4 , 10 Ω external resistance) with visible light and without light. With light, TC molecules were successfully removed (97.3% in 90 min, at initial and optimal pH 5), while generating 0.98 V cell voltage and 24 W m −2 power density, simultaneous removal of COD (chemical oxygen demand) and TOC (total organic carbon) was 91.3% and 95%, respectively, suggesting superior mineralization that can be explained by the excitation of the anodic triple component g-C 3 N 4 /Fe 0 (1%)/TiO 2. In contrast, without light, the removal of COD, TOC and the cell voltage were much lower (48.8%, 65.3%, 0.78 V). In dark, the fuel cell is self-driven and self-biased, forming potential gradient and degrading pollutants. The effects of solution pH, initial TC concentration on degradation and power generation were evaluated. This PFC degrading TC can maintain high photocatalytic activity and high power output capacity after 5 cycles with light. Without light, the electricity generation capacity was 50–70% that in visible light PFC. These features reveal that fuel cell with g-C 3 N 4 /Fe 0 (1%)/TiO 2 photo anode and WO 3 photocathode has great application potential for removing refractory pollutants from wastewater.
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2026
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IF 19.9
Peiyao Bai,Shilin Wei,Qiang Ru,Lang Xu
The development of dynamic electrocatalysts whose active sites evolve under operating conditions represents a frontier in catalysis. An important challenge is to identify suitable pre-catalytic sites and supports that direct dynamic processes toward highly active species while stabilizing them. Here we embed atomically dispersed six-coordinate FeO 6 sites in a 3D-opened multiscale S-doped porous carbon, serving respectively as pre-catalytic sites and supports for electrochemical nitrate reduction to ammonia. During repeated voltammetric scans, the current density increases continuously, revealing dynamic transformation of the FeO 6 sites into residual single-atom sites and newly formed Fe 0 nanoparticles. Integrated in situ and theoretical studies elucidate a dissolution-migration-reduction pathway: deeply embedded FeO 6 single-atom sites dissolve and migrate through interconnected pore channels and are electrochemically reduced to Fe 0 nanoparticles stabilized by the S-doped surface. The dynamically generated Fe 0 nanoparticles show higher nitrate reactivity than the single-atom Fe moieties. Further analysis reveals a crossover mechanism merging the normal and hydroxylamine pathways, accounting for the high ammonia electrosynthesis performance. These findings establish a design principle for dynamic electrocatalysis by pairing a metastable pre-catalytic site with a hierarchically porous sulfur-doped carbon support, converting site evolution from an uncontrolled process into a controllable route for generating and stabilizing highly active species.
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Pei Su,Ge Song,Xuechun Wang,Qizhan Zhang,Wenyang Fu,Minghua Zhou
To improve the mineralization efficiency of pollutants under wide pH ranges by self-sustained electrochemical advanced oxidation processes (EAOPs) without any reagent addition, a flow-through system based on the bifunctional cathode of B, N-doped carbon nanotubes embedded with nano-Fe 0 particles that loaded on graphite felt (Fe@BN-C/GF) was developed. Dominant by 1 O 2 oxidation, the sulfamethazine (SMT) degradation rate and TOC removal in this recirculated flow-through system were 2.6 ∼ 3.3-folds and 1.4 ∼ 2.4-folds that of the batch system under the pH ranges of 3 ∼ 11, respectively. The SMT degradation performance was found not affected in the presence of HCO 3 – , NO 3 – , Cl - , K + , or humic acid (HA). The Fe@BN-C/GF cathode had more potential to treat enlarged wastewater by 5-folds during 10 h operation, and the SMT and TOC removal was 99% and 70.31%, respectively. The total phosphorus (TP), ammonia nitrogen (NH 3 -N) and TOC in reverse osmosis concentrate and secondary wastewater effluent could be simultaneously removed to <0.01 mg L -1 and 8 mg L -1 by this flow-through system with a low electric energy consumption (EEC) of 0.022 and 0.18 kWh gTOC -1 , respectively. This EAOPs based on the flow-through Fe@BN-C/GF cathode was self-sustained, and had very promising application prospect of high mineralization of pollutants even for low-conductivity wastewater.
研究领域:
环境科学
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电化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Chaoyi Zhou,Guojun Lv,Xuyang Zou,Jiangzhang Wang,Yan Chen,Jialing Shen,Shihao Su,Weilong Xing,Deling Fan,Yangbin Shen
Room-temperature ambient air is cheap and easy to obtain, hence the application of room-temperature ambient air as sole oxidant for pollutant degradation is extremely fascinating. In this work, core–shell coordination sponge-Fe 0 @Cu-Pd trimetal catalyst was synthesized via a simple step displacement plating process employing first displacement of Cu and the subsequent displacement of Pd, and applied as heterogeneous catalyst for synergistic catalytic degradation of composite pollutants including TC and PNP. The prepared s-Fe 0 @Cu-Pd trimetal sample was characterized with XRD, SEM, TEM, VSM and XPS. The characterization results revealed the obtained s-Fe 0 @Cu-Pd trimetal sample was a 20 ∼ 30 nm core–shell spherical morphology composed of Fe 0 aggregates core wrapped by a Cu-Pd shell layer. The obtained sponge-Fe 0 @Cu-Pd trimetal catalyst could efficiently activate room-temperature dissolved ambient oxygen and achieve the largest TC removal rate of 99.08 % and PNP removal rate of 97.16 % as well as the biggest removal rate constant of 8.76 min −1 for TC degradation and 7.55 min −1 for PNP degradation within 60 min at experimental conditions: [TC] = 30 mg/L, [PNP] = 30 mg/L, [Catalyst] = 25.52 g/L, pH = 3, 298 K ascribed to the strongest oxidation and reduction ability confirmed by CV characterizations, the lowest charge transfer and contact resistance affirmed by EIS measurements, the strongest O 2 activation ability verified by O 2 -TPD characterizations and DFT analyses, the largest external surface area and mesoporous volume validated by Nitrogen adsorption and desorption characterizations as well as the synergistic catalysis effect for wrapped Cu and Pd. Quenching experiments and EPR characterizations revealed that •OH, •O 2 − , 1 O 2 and •H are all the reactive species and meanwhile •O 2 − served as the main reactive oxygen species. Furthermore, possible mechanisms of TC and PNP degradation via sponge-Fe 0 @Cu-Pd trimetal catalyst were proposed.
研究领域:
环境科学
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催化材料
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污染控制
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
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2018
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IF 5.116
Kané Rabé,Lifen Liu,Noor Ahmed Nahyoon,Yizhen Zhang,Ahmed Mahmoud Idris
Degradation of pollutants can be integrated with electricity generation in Photocatalytic fuel cell under light irradiation or self-powered fuel cell in the dark. In fuel cell driven by electrode reactions , the electrode reduction and oxidation transforms chemical energy in pollutants into electrical energy. In this work, Rhodamine B and coking wastewater were treated, using an efficient Z-scheme g-C 3 N 4 /Fe 0 (1%)/TiO 2 as an anodic catalyst and WO 3 as a cathodic catalyst. After 100 min of reaction in a single chamber fuel cell with 10 Ω of external resistance, in 0.05 M Na 2 SO 4 electrolyte, the paired stainless-steel electrodes loaded respectively with g-C 3 N 4 /Fe 0 (1%)/TiO 2 and WO 3 , degraded 98% Rhodamine B and generated 0.95 V cell voltage under 50 W visible-light irradiation, while removed 60% RhB and generated 0.5 V without light. To investigate the PFC performance of g-C 3 N 4 /Fe 0 (1%)/TiO 2 in treating real coking wastewater, at optimal pH 2, 91% chemical oxygen demand (COD) and 89% total organic carbon (TOC) were removed and generated 0.3 V cell voltage. The influence of pH on photocatalytic degradation performance and cell voltage are evaluated. The high cell voltage is attributed to the very low impedance of the g-C 3 N 4 /Fe 0 (1%)/TiO 2 loaded anode. The excellent electrochemical properties of paired electrodes help in generating higher current density , due to the increased photocatalyst activity of the tridimensional catalyst as proved by electron spinning resonance spectrum, photoluminescence , and Electric Impedance Spectrum analysis.
研究领域:
环境科学
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光催化
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能量转换
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废水处理
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电化学
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材料科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Xiyue Xue,Yanpeng Chen,Yuxin Xiao,Saidi Wang,Hongjie Zhang,Jin Wang,Wen-Hui Zhang
This study pioneers a sustainable “waste-to-wealth” strategy for fabricating a high-performance, pH-universal Fenton-like catalyst (FeCu 2 @BC T4 ) through the one-step co-pyrolysis of acid-precipitated black liquor (APBL) and Fenton sludge with a copper precursor. The innovation lies in the precise engineering of a Fe 0 /Fe 3 O 4 heterojunction synergistically coupled with Cu 0 nanoparticles on a functional APBL-derived biochar. By tuning the Cu/Fe mass ratio and pyrolysis time, the phase composition and electron-transfer properties were optimized. The resulting catalyst exhibits exceptional activity and stability across a broad pH range (3–9), achieving >92.3% methylene blue degradation within 60 min, and demonstrates superior removal efficiency toward various cationic dyes (rhodamine B, crystal violet, malachite green) and an anionic dye (methyl orange). Mechanistic investigations reveal a clear pH-governed transition of reactive oxygen species (ROS) pathways: under acidic conditions (pH 3), •OH-dominated homogeneous–heterogeneous catalysis prevails; under neutral conditions, the system shifts to a heterogeneous process driven by synergistic •OH/ 1 O 2 oxidation. This unique ROS switch is sustained by efficient electron mediation from the biochar matrix, coupled with robust electron supply and transfer enabled by the Fe 0 /Fe 3 O 4 heterojunction and Fe Cu galvanic coupling. This work provides a novel paradigm for converting industrial solid wastes into advanced catalytic materials with a well-elucidated mechanism, effectively overcoming the critical pH limitation of conventional Fenton technologies and showing broad application prospects for organic wastewater remediation.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
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2022
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IF 8.035
Jianan Niu,Xin Kong,Qirui Che,Qingxia Li,Jin Yuan,Jianguo Liu,Yongmei Zhang
Fe 0 above the micro size (zero valent iron; ZVI) can effectively eliminate or inhibit excessive acidification during anaerobic digestion of the organic fraction of municipal solid waste, particularly at high organic loading rates. However, the role of nanoscale ZVI (NZVI) in anaerobic digestion remains controversial. In this study, the effect of NZVI at different dosages (0.4, 0.5, 0.6, 0.7, 0.8 g/g volatile solids [VS]) on the anaerobic digestion stability of the organic fraction of municipal solid waste was investigated and compared with the performance of ZVI, as were its effects on microbial syntrophism. Similarly to ZVI, NZVI recovered methane production from excessive acidification conditions, but the optimal NZVI dosage (0.4 g/gVS) was far lower than that for ZVI (0.8 g/gVS), and eventually the methane yield reached 324 mL/gVS. Microbial structure changes coupled with substance transformation revealed that NZVI enhanced the metabolism of hydrogenotrophic methanogens for interspecies hydrogen transfer and acetotrophic methanogens.
研究领域:
环境工程
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废物管理
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微生物学
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生物技术
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）