ACS Catalysis
·
2023
·
IF 12.9
Heng Shi,Yi He,Yubin Li,Pingya Luo
Fenton-like catalysis based on peroxymonosulfate (PMS) activation has shown great potential in the treatment of organic wastewater. Heterogeneous Fenton-like catalysts containing transition metal active sites are highly efficient for PMS activation. However, the reduction of oxidized metal active sites was usually not prompt due to the sluggish reaction kinetics, which caused the insufficient redox cycle of the metal active sites and further hampered the catalysis efficiency. Recent studies have shown that the synergy effect between photocatalysis and PMS activation may address the above obstacle and boost overall efficiency. However, a deeper understanding of this synergy effect is still missing, making it difficult to be rationally controlled; thus, a poor synergy effect is frequently reported. Herein, a Co/Fe bimetal-doped graphitic carbon nitride (g-C3N4) was designed representatively through systematical characterization and theoretical calculation, the synergy effect was revealed to be profoundly determined by the competitive role of a hole in the system and the adsorbed metastable PMS* on the catalyst surface, and furthermore, the synergy effect can be rationally manipulated; when the Co/Fe doping ratio is 2.5:2.5, the as-prepared g-C3N4 with a moderate valence band position can endow the catalyst with an optimized photo-Fenton-like synergistic effect and the highest catalytic degradation performance. This work sheds light on the rational design of highly efficient photo-Fenton-like catalysts.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Jialu Pan,Lin Che,Tong Wei,Yanqing Cong,Shi-Wen Lv
It is of great significance to rationally regulate the activation mechanism of peroxymonosulfate for wastewater treatment. Herein, for the first time, a newly-constructed NiCo 2 O 4 @ZIF-67 core–shell nanocage was employed as a mediator for effective removal of tetracycline (TC). As-prepared NiCo 2 O 4 @ZIF-67 displayed reduced charge transfer resistance and enhanced electron transfer rate. Importantly, more than 99.58% of TC can be degraded within 30 min by developed NiCo 2 O 4 @ZIF-67/PMS system, and the removal efficiency of TOC was as high as 72.81%. Moreover, antimicrobial tests revealed the low toxicity or non-toxic of degradation products. More interestingly, after coating ZIF-67 film on the surface of NiCo 2 O 4 , the electron transfer process among PMS, contaminant and catalyst was enhanced. The radical and nonradical pathways worked in coordination each other and achieved the rapid removal of various organic pollutants. The ZIF-67-derived NiCo 2 O 4 core dominated the generation of reactive oxygen species, while the coated ZIF-67 shell induced the electron transfer from TC to PMS. Besides, the introduction of ZIF-67 not only improved the anti-interference for inorganic anions, but also boosted the water stability, thereby resulting in that NiCo 2 O 4 @ZIF-67 still remained great catalytic performance after repeated use for several times. In short, current work shared a promising approach for wastewater treatment.
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2023
·
IF 8.8
Yanye Tian,Yu Li,Guang-Guo Ying,Yong Feng
The extensive presence of organic micropollutants in complex water matrices requires the development of selective oxidation technologies . In this study, a novel selective oxidation process was developed via the conjunction of FeMn/CNTs with peroxymonosulfate and successfully used to remove micropollutants such as sulfamethoxazole (SMX) and bisphenol A from aqueous solutions. FeMn/CNTs were prepared using a facile co-precipitation method, characterized using a series of surface characterization techniques, and then tested for pollutant removal . The results showed that the FeMn/CNTs had much greater reactivity than CNTs , manganese oxide , and iron oxide . The pseudo-first-order rate constant with FeMn/CNTs was more than 2.9–5.7 times that of the other tested materials. The FeMn/CNTs had great reactivity in a wide range of pH values from 3.0 to 9.0, with the best reactivity found at pH values of 5.0 and 7.0. High-valent metal-oxo species such as Fe(IV) O and Mn(IV) O and superoxide anion radicals were determined to be the reactive species and were responsible for the oxidation of SMX. These reactive species were selective; therefore, the overall removal performance of SMX was not obviously influenced by high levels of water components including chloride ions, bicarbonates , and natural organic matters. The results from this study may promote the design and application of selective oxidation technologies for micropollutant abatement.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2023
·
IF 5.3
Zhenyu Li,Enhui Du,Panpan Hao,Liyuan Huai,Yang Zhong,Soliman I. El-Hout,Chunlin Chen,Jian Zhang
The oxidation of biomass-derived 5-hydroxymethyl furfural (HMF) into 2,5-Furandicarboxylic acid (FDCA) is a favorable reaction since FDCA is an ideal alternative to petroleum-based monomer terephthalic acid in bio-based polyester industry. However, producing FDCA with high yield under mild conditions is still challenging, especially at energy-saving near-ambient temperatures. Here, we present a Pd nanoparticles catalyst supported on Vulcan XC-72 carbon (Pd/VC) that can completely convert HMF and achieve an encouraging FDCA yield (92.4%) at 30 ℃. The most important observations include yield declines at pure oxygen bubbling, and the transformation of intermediates becomes stagnant; instead, switching to the diluted oxygen is effectively driving the tandem oxidation as the over-oxidation, and thus, rapid deactivation of the Pd surface could be alleviated. The negative effect of high oxygen concentration also occurs in the dehydrogenation and oxygenation of an extended substrate. Since the decisive influence of oxygen content has often been neglected in past investigations of oxidative transformation over Pd-based catalysts, the current study may offer a critical reminder for other liquid-phase oxidation reactions.
✓ 已验证
产品关联
DOI
高影响因子
COLORATION TECHNOLOGY
·
2023
·Vol. 140
·期 2
·300-312
·
IF 1.8
Jianing Fan,Shouying Wu,Zixian Wang,Minglong Zheng,Miaomiao Zhang,Linping Zhang,Yi Zhong,Xiaofeng Sui,Hong Xu,Zhiping Mao
The discharge of coloured textile printing and dyeing wastewater causes environmental pollution. Disposing of wastewater efficiently, simply and with low consumption, is a problem that must be addressed. Herein, a catalytic method for rapid decolorisation of organic dyes was devised employing a terpyridine iron complex to activate oxidised permonosulphate. CI Acid Red 1 was used as the simulated pollutant, the influences of operating parameters on the fading effects of wastewater were explored. According to the results, the produced catalytic system exhibits a universal catalytic effect. Even when the dye concentration reaches 76.4 mg/L, the dyeing wastewater may be effectively decolorised. In addition, when anions (HCO 3 − , SO 4 2− , Cl − ) were present in the solution, the degradation effect of CI Acid Red 1 was still effective. Interestingly, active species such as sulphate radicals and singlet oxygen were detected in the catalytic degradation system by radical capture experiments. The removal rate of total organic carbon can achieve a percentage of 26.22% in 2 hours. This research provides a unique, enzyme-like catalytic system for the rapid breakdown of dye contaminants.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Yuying Chen,Caiwen Wu,Haiyang Xie,Zhaoyan Deng,Yiming Liu,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Tao Gan
Iron-based catalysts have garnered great attention as alternatives for Fenton-like catalysts in the degradation of organic compounds. However, there is a demand for the synthesis of highly efficient iron-based catalysts that can solve the problems of iron dissolution and poor stability. Herein, nitrogen-doped graphitic carbon-supported Fe-Co/Fe 3 C dual active sites catalyst (Fe-Co/Fe 3 C-NC) is successfully prepared by ball milling method combined with subsequent high-temperature self-reduction. 0.5 wt%-Fe-Co/Fe 3 C-NC shows high efficiency in the activation of peroxymonosulfate (PMS) for the ultrafast degradation of high concentration Rhodamine B (200 mg/L of RhB is completely degraded within 8 min and the degradation rate constant is as high as 0.5066 min −1 ), as well as high stability and good reproducibility, attributing to the synergistic mechanism between the dual active sites (Fe-Co and Fe 3 C) and the adsorption sites (Fe 3 C and pyrrolic-N). Chemical quenching experiments and electron paramagnetic resonance indicate that the prepared 0.5 wt%-Fe-Co/Fe 3 C-NC exhibits outstanding activation for PMS by generating reactive oxygen species (SO 4 •− , • OH, 1 O 2 ) and high-valent FeCo=O species. This work shows useful insights into the synthesis of iron-based dual active sites catalysts, providing exciting chances for the highly efficient degradation of high concentration organic wastewater.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xinyu Song,Yang Shi,Zelin Wu,Bingkun Huang,Xinhao Wang,Heng Zhang,Peng Zhou,Wen Liu,Zhicheng Pan,Zhaokun Xiong,Bo Lai
The discriminative activities and mechanisms for activation of O-O bond in peroxy compounds via single-atom catalysts (SACs) especially with a higher coordination number (M-N 5 ) are rarely explored. Herein, the atomic catalyst (Fe-SAC) with Fe-N 5 as the active center was constructed, which could simultaneously and effectively activate peroxymonosulfate (PMS), peroxydisulfate (PDS), and hydrogen peroxide (H 2 O 2 ). Density functional theory (DFT) calculations combined with experiments results demonstrated that the degradation efficiencies of acyclovir were corresponding to the changes of O-O bond length in various peroxy compounds. Meanwhile, the experiments exposed that the three oxidants all produced • OH, but the PMS also contained 1 O 2 and Fe(IV)=O, and PDS contained O 2 •- additively. The scale-up experiment showed Fe-SAC could operate steadily for nearly 7 d. Overall, this work unveils the discriminative mechanisms for activation of O-O band in different Fenton-like systems. Moreover, the Fe-SAC with high coordination numbers has excellent catalytic properties and practical performance.
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2023
·
IF 10.9
Yang Zhao,Biao Ma,Xiaomei Liu,Ning Li,Yang Li,Xiaobin Fan,Wenchao Peng
Recently, single atomic metals supported on carbon materials have attracted great interests because of their high catalytic activity and stability in peroxymonosulfate (PMS)-based Fenton-like process. Herein, we propose a convenient strategy to synthesize Co single atoms supported on nitrogen-doped carbon spheres (Co@MNC) via microwave treatment. The microwave irradiation can simultaneously induce the formation of carbon defects and immobilize the Co single atoms in N doped carbon support in a few minutes. The obtained Co@MNC can activate PMS for efficient catalytic oxidation of organic pollutants. The radical quenching tests and electron paramagnetic resonance (EPR) verify that Co (IV)-oxo species, 1 O 2 , and O 2 •− are responsible for the remediation of organic pollutants. Density functional theory (DFT) calculations confirm that unique and low coordinated Co–N 2 on void or edge defects are favorable for PMS adsorption. The electrons will then transfer from Co atoms to adsorbed PMS via the bonded N. Co (IV)-oxo species and other ROSs are therefore generated for pollutants degradation. This work provides a fast method for the synthesis of single atom catalysts for efficient Fenton-like reactions.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Haiqing Zhang,Richard Lee Smith,Haixin Guo,Xinhua Qi
Ordered mesoporous carbons (OMCs) functionalized with catalytically-active metals have many potential applications in sulfate radical-based advanced oxidation processes for degrading antibiotics. Cobalt cross-linked ordered mesoporous carbon materials (OMC-Co-Tx) were synthesized through evaporation-induced self-assembly, calcinated at (600 to 800) o C. The OMC-Co-Tx materials were then employed as peroxymonosulfate (PMS) activators for removal of sulfamethoxazole (SMX) from aqueous solutions. OMC-Co-T800 prepared by calcination at 800 °C had a large specific surface area (449 m 2 /g), uniform pore structure (∼4.5 nm) and showed the best performance for activation of PMS. With a dosage of 0.1 g/L OMC-Co-T800 and 0.4 g/L PMS, the functionalized OMC material allowed SMX (10 mg/L) removal of up to 99% in 30 min. The increase of calcination temperature promoted the reduction of cobalt in OMC materials and increased the defects in their structure, resulting in better catalyst behavior. Quenching experiments and electron paramagnetic resonance analyses showed that reactive species of sulfamethoxazole degradation involved in the OMC-T800/PMS system were SO 4 •− , OH, O 2 •− and 1 O 2 . HPLC-MS analyses of degradation intermediates formed in the OMC-Co-T800/PMS system allowed elucidation of four transformation pathways for SMX degradation.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ping Zhang,Mingxue Xiang,Wei Jiang,Huiling Liu,Yu Chen,Ying Fang,Longyong Wu,Hongjun Guo,Yufei Wang
Integrated adsorption and photocatalysis is a worth frontier strategy for recalcitrant organics elimination, yet the current challenge is developing materials featured with dual functions of adsorption/photocatalytic ability. In this scenario, a novel attractive exfoliated vermiculite coupling with Cu(II) composite (eVT@Cu) was tactfully engineered. Specifically, exfoliated structure containing vast negative charge was conductive for Cu(II) loading. The anchored Cu(II) played triple roles in this system, that is, regulating electron configuration of photocatalyst with narrow bandgap, as well as providing complexation sites for tetracycline (TC) enrichment. With the help of inherent Fe(III), Cu(II) was readily to form heterogeneous high-valence Cu(III) driven by photonic energy. Benefited by these effects, eVT@Cu exhibited extremely augment on TC removal compared to pristine VT and eVT, with ca. 80% removal efficiency through the synergy of adsorption and photocatalysis. Overall, this study not only provides an excellent environmental candidate for TC removal but also opens a brand-new perspective for the generation of heterogeneous high-valence Cu(III) over eVT@Cu under visible light.
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2023
·Vol. 13
·期 9
·1246
·
IF 3.9
Jianhui Zhao,Huan Li,Yuanzhou Wang,Jingjie Yu,Ning Li,Shaopo Wang
Biochar (BC) usually has abundant surface functional groups, well-developed pore structures and high specific surface areas, which can combine with transition metals for peroxymonosulfate (PMS) activation to degrade organics. In this paper, BC modified with Cu/CuO was prepared by a modified impregnation pyrolysis method using peanut shells as raw materials. The morphology, structure and physicochemical properties were analyzed. Results showed that the originally smooth BC surface was modified into a rough structure with distributed metal particles, and the specific surface area of the modified Cu/CuO-BC700 (i.e., Cu/CuO-BC) increased from the initial 22.57 to 192.64 m2/g. The Cu/CuO-BC was employed for PMS activation and tetracycline (TC) degradation, achieving a removal efficiency of 93.2% at TC initial concentration 20 mg/L, PMS concentration 0.5 mM and catalyst dosage 0.1 g/L after 30 min. The influence of co-existing anions in the actual water on TC degradation followed the order of HCO3−> H2PO4−> Cl−, and HA had an inhibitory effect on TC degradation. A variety of active species participated in TC degradation, and the free radical pathway played a dominant role. Furthermore, the Cu/CuO-BC could maintain the degradation efficiency of TC up to 80% even after five consecutive cycles. The Cu/CuO-BC maintained high activity through redox reactions between catalytically generated active species and the cycling of metal ions (Cu+/Cu2+).Keywords:Cu/CuO;modified biochar;peroxymonosulfate;active species;tetracycline
✓ 已验证
产品关联
DOI
高影响因子
Journal of Water Process Engineering
·
2023
·
IF 7
Fuwang Zhao,Yanling Yang,Siyang Ji,Rui Yu,Xing Li,Zhiwei Zhou
A photo-Fenton catalyst Fe‑carbon nitride (g-C3N4)/reduced graphene oxide (rGO) (labeled as FNGO) was prepared via two-step calcination thermal polymerization. rGO as a carrier of Fe-g-C3N4 accelerated the charge transfer and improved the reduction of Fe (III) as compared those of the binary Fe-g-C3N4 catalyst. The FNGO catalyst maintained a high surface area of 264.7 m2/g and its charge transfer rate was 2.77 times higher than Fe-g-C3N4. The decreasing transient photocurrent and increasing electrode resistance of FNGO, Fe-g-C3N4 and g-C3N4 confirm the positive synergistic effect of Fe N coordination and rGO in charge transfer. Under the synergistic of visible light irradiation and H2O2, the excellent degradation performance of FNGO towards rhodamine B was achieved (95.3 % removal) at Fe-doping content of 10 wt%, rGO loading content of 0.5 % and H2O2 addition of 1.5 mM. Hydroxyl radicals played a dominant role in the photocatalysis-Fenton system, which was related to the coordination of Fe N, the carrier off-domain of rGO, and the Fe (III)/Fe (II) cycle promoted by photogenerated electron and superoxide radicals. The FNGO had a high stability, a wide pH adaptation (3– 11) and a low Fe-leaching. This novel ternary light-driven photo-Fenton catalyst of FNGO enabled efficient decontamination during advanced treatment of wastewater.
✓ 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）