JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Jiabao Wu,Ying Tao,Chi Zhang,Qiong Zhu,Dieqing Zhang,Guisheng Li
Photoelectrochemical (PEC) activation of chloride ions (Cl - ) to degrade persistent organic pollutants (POPs) is a promising strategy for the treatment of industrial saline organic wastewater. However, the wide application of this technology is greatly restricted due to the general photoanode activation of Cl - with poor capability, the propensity to produce toxic by-products chlorates, and the narrow pH range. Herein, oxygen vacancies-enriched titanium dioxide (O v -TiO 2 ) photoanode is explored to strongly activate Cl - to drive the deep mineralization of POPs wastewater in a wide pH range (2−12) with simultaneous production of H 2 . More importantly, nearly no toxic by-product of chlorates was produced during such PEC-Cl system. The degradation efficiency of 4-CP and H 2 generation rate by O v -TiO 2 were 99.9% within 60 min and 198.2 μmol h −1 cm −2 , respectively, which are far superior to that on the TiO 2 (33.1% within 60 min, 27.5 μmol h −1 cm −2 ) working electrode. DFT calculation and capture experiments revealed that O v -TiO 2 with abundant oxygen vacancies is conducive to the activation of Cl - to produce more reactive chlorine species, evidenced by its high production of free chlorine (48.7 mg L −1 vs 7.5 mg L −1 of TiO 2 ). The as-designed PEC-Cl system in this work is expected to realize the purification of industrial saline organic wastewater coupling with green energy H 2 evolution.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Wenjie Kuang,Zhang Yan,Jinxiu Chen,Xiaotang Ling,Wenxiao Zheng,Weijun Huang,Chunhua Feng
Electrochemical oxidation has been demonstrated to be a useful method for removing biorefractory organic pollutants in mature landfill leachate but suffers from low efficiency in eliminating ammonium because of its resistance to being oxidized by HO• or free chlorine (FC) at decreased pH. Here, we propose a new bipolar membrane-electrochlorination (BPM-EC) process to address this issue. We found that the BPM-EC system was significantly superior to both the undivided and divided reactors with monopolar membranes in terms of elevated rate of ammonium removal, attenuated generation of byproducts (e.g., nitrate and chloramines), increased Faradaic efficiency, and decreased energy consumption. Mechanistic studies revealed that the integration of BPM was helpful in creating alkaline environments in the vicinity of the anode, which facilitated production of surface-bound HO• and FC and eventually promoted in situ generation of ClO•, a crucial reactive species mainly responsible for accelerating ammonium oxidation and selective transformation to nitrogen. The efficacy of BPM-EC in treating landfill leachates with different ammonium concentrations was verified under batch and continuous-flow conditions. A kinetic model that incorporates the key parameters was developed, which can successfully predict the optimal number of BPM-EC reactors (e.g., 2 and 5 for leachates containing 589.4 ± 5.5 and 1258.1 ± 9.6 mg L–1 NH4+-N, respectively) necessary for complete removal of ammonium. These findings reveal that the BPM-EC process shows promise in treating ammonium-containing wastewater, with advantages that include effectiveness, adaptability, and flexibility.
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WATER RESEARCH
·
2022
·
IF 13.4
Wenxiao Zheng,Yingkai Chen,Hengyi Fu,Zhang Yan,Zhenchao Lei,Weijian Duan,Chunhua Feng
The generation of chlorinated byproducts during the electrochemical oxidation (EO) of Cl − -laden wastewater is a significant concern. We aim to propose a concept of converting reactive species (e.g., reactive chlorines and HO • resulting from electrolysis) into 1 O 2 via the addition of H 2 O 2 , which substantially alleviates chlorinated organic formation. When phenol was used as a model organic compound, the results showed that the H 2 O 2 -involving EO system outperformed the H 2 O 2 -absent system in terms of higher rate constants (5.95 × 10 −2 min −1 vs. 2.97 × 10 −2 min −1 ) and a much lower accumulation of total organic chlorinated products (1.42 mg L −1 vs. 8.18 mg L −1 ) during a 60 min operation. The rate constants of disappearance of a variety of phenolic compounds were positively correlated with the Hammett constants ( σ ), suggesting that the reactive species preferred oxidizing phenols with electron-rich groups. After the identification of 1 O 2 that was abundant in the bulk solution with the use of electron paramagnetic resonance and computational kinetic simulation, the routes of 1 O 2 generation were revealed. Despite the consensus as to the contribution of reaction between H 2 O 2 and ClO − to 1 O 2 formation, we conclude that the predominant pathway is through H 2 O 2 reaction with electrogenerated HO • or chlorine radicals (Cl • and Cl 2 • − ) to produce O 2 • − , followed by self-combination. Density functional theory calculations theoretically showed the difficulty in forming chlorinated byproducts for the 1 O 2 -initiated phenol oxidation in the presence of Cl − , which, by contrast, easily occurred for the Cl • -or HO • -initiated phenol reaction. The experiments run with real coking wastewater containing high-concentration phenols further demonstrated the superiority of the H 2 O 2 -involving EO system. The findings imply that this unique method for treating Cl − -laden organic wastewater is expected to be widely adopted for generalizing EO technology for environmental applications.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Jie Zhou,Hao Liu,Chao Xiong,Peng Hu,Hao Wang,Xuyu Wang,Hongbing Ji
Propane dehydrogenation (PDH) has been a promising method to satisfy the increasing demand for propylene, but Pt-based catalysts always suffer from sintering and coke formation. Developing stable and efficient catalysts for PDH is of great significance for the industry. Herein, the paper reports that a catalyst with potassium-promoted Pt-In bimetallic clusters encapsulated in silicalite-1 (S-1) zeolite works as an efficient and stable catalyst for PDH. The catalyst achieves a propane conversion of 43.73 % with 97.14 % selectivity of propene and an extremely high propylene productivity of 20.33 mol g Pt -1 h -1 with a weight hourly space velocity (WHSV) of 6.75 h −1 . No obvious deactivation occurs after 48 h on stream, affording an extremely low deactivation constant of 0.0025 h −1 . The introduction of indium species greatly improves the propene selectivity and restricts the coke formation. The introduction of K + into S-1 can significantly enhance the catalytic activity and the stability of the catalyst. The catalyst with excellent activity and stability is potential for industrial application.
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Reaction Kinetics Mechanisms and Catalysis
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2022
·Vol. 135
·期 5
·2565-2578
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IF 1.843
Cai Zhaotian,Guo Xiaoxuan,Zhang Lixiang,Xiao Guomin
This work reports the synthesis of Zinc porphyrin-based porous (POP-ZnTPP) by a typical Yamamoto-Ullmann coupling reaction, which exhibited abundant tiny nanopores, excellent CO 2 adsorption capacity, and CO 2 /N 2 selectivity. The open pore environment of POP-ZnTPP facilitated the exposure of active sites, which intensified the catalytic activity in the cycloaddition reaction of epoxides (PO) with CO 2 under mild conditions. As expected, POP-ZnTPP catalyst completely converted PO to cyclic carbonates (COCs) at ambient temperature (25 °C, 1.5 MPa). It is also worth noting that POP-ZnTPP could convert PO into COCs under the simulated flue gas (15% CO 2 and 85% N 2 , v/v) atmosphere, which is very favorable for industrial applications of CO 2 . In addition, POP-ZnTPP catalyst as one of the most outstanding catalysts exhibited excellent broad substrate scope and remarkable reusability. This work has a certain guiding significance for developing an environmentally friendly COC production process.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Xianhu Long,Zhaokun Xiong,Rongfu Huang,Yahan Yu,Peng Zhou,Heng Zhang,Gang Yao,Bo Lai
Herein, an electrochemical (EC) system was applied as “co-catalyst” to enhance the activation of peroxymonosulfate (EC/Fe(III)/PMS) for efficient Sulfamethoxazole (SMX) degradation. The cathodic reduction reaction can facilitate electron transfer to Fe(III) and trigger the sustainable Fe(III)/Fe(II) redox cycle. Unexpectedly, in addition to hydroxyl radical ( OH) and sulfate radical (SO 4 •− ), non-radicals mechanism including singlet oxygen ( 1 O 2 ) and Fe(IV) were also found involved in EC/Fe(III)/PMS system. The degradation of SMX in EC/Fe(III)/PMS system was accomplished by the collaboration of radicals and non-radicals oxidation . The generation routes and mechanisms of involved reactive oxygen species (ROS) were explored. The relative contributions of OH, SO 4 •− , and nonradical species for the degradation of SMX were calculated to 4.75 %, 25.31 %, and 69.94 %, respectively. Besides, multiple degradation pathways of SMX were proposed by identifying the formed byproducts. The EC/Fe(III)/PMS process could efficiently degrade SMX under the influence of co-existing ions and inactivate pathogens in the wastewater.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
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IF 14.224
Zhenchao Lei,Ziyuan Huang,Yimin Lin,Yuwei Liu,Zhang Yan,Wenxiao Zheng,Huanxin Ma,Zhi Dang,Chunhua Feng
The corrosion of Fe(0) in the presence of O 2 in nature can lead to the oxidation of organic compounds, but the efficiency is very limited. Herein, attempts were made to establish a galvanic system that separates the anodic Fe(0) oxidation reaction and the cathodic O 2 reduction reaction using an air-breathing cathode. Compared with the chemical Fe(0)/O 2 system, it exhibited a substantially higher capability of destroying a variety of pollutants, such as organic dyes (12 types), phenol , nitrobenzene , acetaminophen, phenol, and ethylenediaminetetraacetic acid. The degradation rate constant of a model dye (i.e., Rhodamine B) increased from 0.047 min − 1 (chemical) to 1.412 min −1 (galvanic) under the passive air-breathing condition. The electric circuit design promoted Fe(0) dissolution to Fe(II) and triggered electron transfer that drives O 2 reduction to H 2 O 2 , two important species responsible for the generation of HO • at high abundance. In addition, the galvanic Fe(0)/O 2 system produces electricity while destroying pollutants. Tests with real Ni plating wastewater further demonstrated the capability of the system to oxidize complexed organics and phosphite. This study provides a new strategy for boosting the oxidative capacity of the Fe(0)/O 2 system, which shows promise for acid wastewater treatment .
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2022
·
IF 7.926
Sai Zhang,Ruoning Guo,Ming Liang,Li Li
ZnFe 2 O 4 (ZFO) poses great potential to activate peroxymonosulfate (PMS) and responds to visible light. In this work, ZFO was synthesized by a simple one-step hydrothermal method . In order to obtain the most desirable photoelectric performance, hydrothermal reaction parameters including pH, temperature, and time were innovatively regulated. Based on optimized ZFO, the visible light/PMS/ZFO (Vis/PMS/ZFO) system was established, which presented superior degradation efficiency of ciprofloxacin (CIP). It was verified that •OH and 1 O 2 were the main reactive species for CIP degradation. Besides, visible light was confirmed to promote formation of reactive species and accelerate charge transfer simultaneously. Therefore, the possible mechanism of catalysis was proposed and the enhancement of visible light for the PMS/ZFO system was elaborated. Based on the identified intermediates, three pathways of CIP degradation were illustrated. Moreover, water matrix posed an overall positive impact on CIP degradation. Experiments performing in real wastewater and repeated tests validated wide application of the Vis/PMS/ZFO system. In general, the designed synthesis of ZFO is feasible and the integration of ZFO with visible light for efficient PMS activation is a successful and promising method for wastewater treatment .
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WATER RESEARCH
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2022
·
IF 13.4
Yan Xia,Xinbai Jiang,Yuxuan Wang,Qian Huang,Dan Chen,Cheng Hou,Yang Mu,Jinyou Shen
Anaerobic technology is extensively applied in the treatment of industrial organic wastewater, but high salinity always triggers microbial cell dehydration, causing the failure of the anaerobic process. In this work, betaine, one kind of compatible solutes which could balance the osmotic pressure of anaerobic biomass, was exogenously added for enhancing the anaerobic reduction of nitrobenzene (NB) at high salinity. Only 100 mg L −1 betaine dosing could significantly promote the removal efficiency of NB within 35 h at 9% salinity (36.92 ± 4.02% without betaine and 72.94 ± 6.57% with betaine). The relieving effects on salt stress could be observed in the promotion of more extracellular polymeric substances (EPS) secretion with betaine addition. Additionally, the oxidation-reduction potential (ORP), as well as the electron transfer system (ETS) value, was increased with betaine addition, which was reflected in the improvement of system removal efficiency and enzyme activity. Microbial community analysis demonstrated that Bacillus and Clostridiisalibacter which were positively correlated with the stability of the anaerobic process were enriched with betaine addition at high salinity. Metagenomic analysis speculated that the encoding genes for salt tolerance ( kdp B /oad A /bet A /opu D /eps P /eps H) and NB degradation ( nfs A /wrb A /ccd A /men C) obtained higher relative abundance with betaine addition under high salt environment, which might be the key to improving salt tolerance of anaerobic biomass. The long-term assessment demonstrated that exogenous addition betaine played an important role in maintaining the stability of the anaerobic system, which would be a potential strategy to achieve a high-efficiency anaerobic process under high salinity conditions.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Tong Liu,Yang Liu,Peng Zhou,Zhaokun Xiong,Heng Zhang,Chuanshu He,Ye Du,Gang Yao,Bo Lai
As one of the most promising advanced oxidation processes , the activation of S(IV) by iron-based materials to produce SO 4 •− has become a hot technology for the degradation of organic pollutants . However, the mechanism of radical chain reactions has not been clearly explored. Herein, we established a novel AOP system based on the combination of zero-valent iron (ZVI) and potassium pyrosulfite (PPS). Combined with the degradation trends of CBZ and the change of DO concentration, the system was proposed to be divided into a slow initiation stage in 5 min and a rapid degradation stage in 5 − 10 min. Through a series of quenching experiments, electron paramagnetic resonance tests and several probe experiments, the mechanisms of two radical chain reactions were proposed between ZVI and PPS: the first one produced O 2 •− and HO • , and the other produced SO 3 •− , SO 5 •− , SO 4 •− and HO • . The two-stage reaction and two radical production paths of the ZVI/PPS system were proposed for the first time, which provided theoretical guidance for the practical application of the ZVI/PPS system. The ZVI/PPS system has been found to have excellent environmental adaptability in the treatment of industrial wastewater .
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JOURNAL OF CATALYSIS
·
2022
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IF 8.047
Lihua Zhu,Huan Zhang,Huaze Zhu,Huan Fu,Anna Kroner,Zhiqing Yang,Hengqiang Ye,Bing Hui Chen,Rafael Luque
Herein, we report a simple synthesis of PtNiCo trimetallic nanoparticles (NPs) loaded on carbon black (PtNiCo/C) via ambient-temperature chemical reduction and galvanic replacement reaction. The influence of thermal treatment temperature in 10 %H 2 /N 2 on PtNiCo NPs in PtNiCo/C-X nanostructures is revealed, where, X = 200 °C, 500 °C. XRD, XPS, TEM, HAADF-STEM, HRTEM, STEM-EDX elemental line-scanning (mapping), HS-LEIS, H 2 -TPR, atomic resolution aberration-corrected STEM (AC-STEM), XANES and EXAFS have been employed to characterize various nanostructures of PtNiCo NPs in PtNiCo/C-X. We established the relationship of nanostructure-reducing temperature thus catalytic behavior of PtNiCo/C-X: PtNiCo/C-200 ∼ Pt island (single atom and cluster)-on-NiCo alloy NP, PtNiCo/C-500 ∼ PtNiCo alloy NPs. PtNiCo/C-200 provides much improved catalytic activity and selectivity to target products ( NO 2 group hydrogenation) as compared to PtNiCo/C-500 for nitroarenes selective hydrogenation under mild reaction conditions (1.0 MPa-H 2 pressure, 18 °C or 40 °C-reaction temperature). That is considered to be closely correlated with the synergy effect of Pt islands and NiCo alloy nanoparticles in PtNiCo/C-200.
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JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Jiansong Wang,Yangyang Yu,Wenkai Xu,Hui Yu,Weiwei Zhang,Hongliang Huang,Gui-Rong Zhang,Donghai Mei
Ammonia borane (AB) represents a promising hydrogen storage material, while high-performing catalysts allowing efficient release of hydrogen from the hydrolysis of AB are desired. Here, Pd nanoclusters (NCs) are successfully immobilized within pores of a bipyridyl covalent triazine framework (CTF-BPDA-TPDH) via a metal-nitrogen coordination reduction strategy. The porous structure and tailored N sites of CTF facilitate the anchoring of Pd ions and the in situ formation of monodisperse Pd NCs confined in the pores of CTF. The resulting Pd-NCs@CTF composites exhibit high activity toward the hydrolysis of AB with turnover frequencies (TOFs) of 273 and 434 mol H2 ·mol −1 Pd ·min −1 in neutral and alkaline solutions, respectively. The Pd-NCs@CTF catalyst is also demonstrated for the tandem dehydrogenation of AB and hydrogenation of nitroarenes featuring short reaction time and high yields. These findings emphasize the promise of the porous CTFs encapsulated metal NCs for active catalysts.
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