Desalination and Water Treatment
·
2024
·
IF 1
Yulu Zhang,Jiping Jia,Nanxin Chang,Yuzeng Zhao,Xinjing Meng,Honghua Ge
The development of cheap and efficient catalysts for persulfate activation in advanced oxidation processes based on persulfate is important and promising in the wastewater treatment field. Herein, conductive carbon black loaded CuFe 2 O 4 (CCB-CuFe 2 O 4 ) had been prepared via a sol-gel method and was used as a catalyst to activate persulfate for the removal of phenol in water. The CCB-CuFe 2 O 4 was characterized by X-ray diffraction, Fourier-transform infrared spectroscopy, Brunauer–Emmett–Teller, and Raman spectroscopy, which confirmed that CuFe 2 O 4 nucleated on the defect of CCB. The performance of the activation on persulfate was studied by determining the concentration of phenol and chemical oxygen demand of the water. The activity of the catalyst is the highest when the content of CuFe 2 O 4 in the catalyst is 10%. The removal rate of 100 mg/L phenol reached 100% in 30 min under the optimized operation condition, which was 2.0 g/L CCB-CuFe 2 O 4 , 2.0 mmol/L persulfate (PS) and pH = 11. The factors of effect on the catalysis performance were discussed. CCB-CuFe 2 O 4 can be used in the pH range of 3~11 and the presence of HCO 3 – can promote phenol degradation rate. The use of CCB-CuFe 2 O 4 catalyst obviously reduced the dose of PS in the process of phenol oxidation degradation. Furtherly, quenching experiments verified that the most important reactive species in the CCB-CuFe 2 O 4 /PS/phenol system is singlet oxygen ( 1 O 2 ).
研究领域:
环境科学
·
催化化学
·
水处理技术
✓ 已验证
DOI
高影响因子
ACS Applied Engineering Materials
·
2023
·
IF 0
Yuchao Chen,Li Wang,Yufei Shu,Qi Han,Beizhao Chen,Mengxia Wang,Xun Liu,Danyal Rehman,Bei Liu,Zhongying Wang,John Lienhard
The economic value of recovering gold from electronic waste (e-waste) has generated significant interest, but selective capture of gold from complex acidic electronic leaching solutions remains challenging. Here, we synthesized poly-m-phenylenediamine (PmPD) nanoparticles with a positively charged surface and amino functional groups, resulting in an adsorption capacity of 2063 mg/g for Au(III) in acidic solutions, superior to most traditional adsorbents. Electrostatic adsorption and reduction were identified as the adsorption mechanism for Au(III) by zeta potential, X-ray diffraction, transmission electron microscope, Fourier transform infrared, and X-ray photoelectron spectroscopy analyses. To enable adsorbent recycling, PmPD nanoparticles were assembled into adsorptive membranes and used for gold recovery from e-wastewater via a continuous-flow membrane separation process. The PmPD membrane achieved a dynamic gold recovery capacity of approximately 530 mg/g and could be effectively regenerated after washing with a mixture of thiourea and HCl. We demonstrated the practical application of the adsorptive membranes by recovering about 100% of gold from the leaching solution of waste printed circuit boards of computers. Finally, the recovered gold nanoparticles on the PmPD membrane were used to catalyze the degradation of p-nitrophenol, showcasing the catalytic property of gold. The Au@PmPD membrane loaded with 4 mg gold exhibited a high catalytic reduction performance with an apparent rate constant of 0.59 min–1, one of the highest catalytic degradation rate constants of p-nitrophenol reported to date. Our study presents an effective and economical approach for recovering gold from e-waste, providing a prototype of resource recovery and reuse.
研究领域:
环境科学
·
材料科学
·
化学工程
·
资源回收
·
催化作用
✓ 已验证
DOI
ENVIRONMENTAL POLLUTION
·
2018
·
IF 4.358
Zhaocheng Zhang,Dongyang He,Haiyang Liu,Miao Ren,Yanan Zhang,Jiao Qu,Nan Lu,Jiunian Guan,Xing Yuan
Black phosphorus (BP), a superior two-dimensional (2D) semiconductor, has attracted much attention due to its unique properties. The graphene (GR)-BP hybrid was synthesized through one pot chemical vapor transport (CVT) approach. The characterization results indicated that P atom was successfully incorporated into GR by the formation of P-C bond. Remarkably, the newly-synthesized GR-BP represented high photocatalytic activity towards 2-chlorophenol (2-CP) degradation, due to the high efficiency of charge separation and transformation caused by the direct band gap of BP and carrier mobility of GR. The removal efficiency for 2-CP reached up to 87.08% within visible light irradiation for 180 min ( λ > 420 nm). The degradation rate of GR-BP hybrid for 2-CP was approximately 7.29-fold than that of BP within 30 min. In addition, the little increasing of the peak for P-O bond in GR-BP hybrid was observed after being exposed in air for 15 days, meant that the stability of BP was significantly enhanced. It was caused by the decreasing of the oxidation sites in BP due to the formation of P-C bond in hybrid. In brief, our synthetic method for GR-BP not only provides a novel route for the improvement of the stability of BP, but also constitutes an insight into the promising practical application of BP in the photocatalysis field.
研究领域:
材料科学
·
纳米科技
·
光催化
·
半导体材料
·
环境化学
✓ 已验证
DOI
高影响因子
WATER SCIENCE AND TECHNOLOGY
·
2020
·Vol. 82
·期 4
·704-714
·
IF 1.638
Sun Jie,Xia Guotong,Yang Wenjin,Hu Yue,Shen Weibo
The radical generation properties of hydrogen peroxide and persulfate for phenol degradation were investigated under microwave irradiation using copper-doped silicon carbide (Cu/SiC) composites as catalyst. The results showed that 90% and 70% of phenol and total organic carbon (TOC), respectively, were removed within 7 min. Microwave activation of hydrogen peroxide and sodium persulfate in terms of thermal effects and accelerated electron transfer was analyzed by degradation kinetics and X-ray photoelectron spectroscopy (XPS). The microwave activation of Na 2 S 2 O 8 demonstrated that the hot spots promote decomposition of persulfate more rapidly and the rate of persulfate decomposition was more than three times the activation rate of a normal heating method. There is a synergistic effect between Cu and microwave radiation, which is highlighted by the H 2 O 2 activation; ·OH was generated due to the redox cycle between Cu(I)/Cu(II) and was responsible for phenol degradation using H 2 O 2 . High performance liquid chromatography (HPLC) analysis indicated that hydroxylation and sulfate radicals addition of phenol were the initial oxidation reaction steps of hydrogen peroxide and persulfate, respectively, followed by further oxidation to form short-chain carboxylic acids. The kinetic advantages of microwave-assisted reactions. The activation of persulfate involved thermal gradients and redox reaction simultaneously. The reaction mechanism in Na 2 S 2 O 8 -Cu/SiC system was examined.
研究领域:
环境科学
·
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Qingqing Shi,Yaqi Hou,Qiting Zhu,Yongmei Hao
Due to the complex structure of metal–carbon-based catalysts derived from metal-organic frameworks (MOFs), it is difficult to clarify the active sites and catalytic mechanisms. Constructing of structure–activity relationship is conducive for identifying active center, but there is still a gap in the bimetal-carbon-based catalysts/PMS systems. Here, we report a highly efficient and stable CuCo bimetal-nitrogen doped carbon catalyst (CuCo@C-N) for the activation of PMS for efficient degradation of PNP. By manipulating the catalyst structure, establishing the structure–activity relationship and combining with DFT calculation, the non-metallic active centers were determined, including defects, C=O and graphite N. Co was the only metal active center, and the presence of Cu accelerated the redox cycle of the system. The degradation of PNP was dependent on electron transfer and ROS activation. The metal active center was used to generate sulfate radicals (SO 4 •− ), and the non-metal active sites accelerated electron transfer and non-radical pathways to generate 1 O 2 .
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL ENGINEERING
·
2024
·Vol. 150
·期 8
·04024038
·
IF 1.6
Jingcheng Wei,Jing Zhang,Bingyan Zhu,Tingfeng Xue,Zejia Song,Sumin Li,Liwei Pan
Activation of peroxymonosulfate (PMS) by catalysts for water treatment is very important for the sulfate radicals-based advanced oxidation technology. Constructing affordable and recyclable transition metal catalysts with high efficiency is highly desirable, but still challenging. In this study, a novel CoAl2O4/Co2O3@γ-Al2O3 catalyst for the activation of PMS was prepared with an excessive impregnation method, and its performance on the catalytic degradation of phenol in water was investigated. The composition and structure of the catalyst were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, and N2 adsorption-desorption experiments. It was found that the catalyst could greatly promote the phenol mineralization in water as the total organic carbon removal increased from 4.27% to 57.64% after 60 min of reaction. The presence of Cl− inhibited the catalytic degradation of phenol in water at low concentrations, but promoted the catalytic degradation at high concentrations. However, HCO3− and CO32− revealed inhibitory effects on the catalytic degradation because they could scavenge free radicals in the system. Based on the electron spin resonance technique and the quenching experiments, O12 and SO4−· were identified to be the primary reactive species for the catalytic degradation. The CoAl2O4/Co2O3@γ-Al2O3 could be easily recovered and reused. The toxicity evaluation verified that the toxicity of the treated water was greatly decreased after the catalytic degradation. Therefore, the CoAl2O4/Co2O3@γ-Al2O3 prepared in this study could be an effective catalyst for the catalytic degradation of phenol in water by activating PMS.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 34
·27043-27051
·
IF 3.84
Weiqian Pan,Guangshan Zhang,Tong Zheng,Peng Wang
CuO/Al2O3 was synthesized successfully by the impregnation-deposition method and used as a heterogeneous catalyst in a microwave assisted Fenton-like process (MW/FL). The morphology and physico-chemical properties of the CuO/Al2O3 catalyst were characterized using field emission scanning electron microscopy (FESEM), X-ray diffraction (XRD) and Brunauer–Emmett–Teller (BET) analysis. The degradation of p-nitrophenol (PNP) was investigated by different processes, including microwave irradiation (MW) alone, hydrogen peroxide (H2O2) oxidation under microwave irradiation without the catalyst (MW/H2O2), a Fenton-like (FL) process, a MW/FL process and a thermally-assisted Fenton-like (TH/FL) process. The results showed that the CuO/Al2O3 catalyzed MW/FL could generate more hydroxyl radicals (˙OH) and remove PNP more effectively compared to other processes. The effects of initial pH, dosage of H2O2 and catalyst, microwave power and radiation time, and PNP concentration on the removal efficiency were also studied. The results showed that 93% removal efficiency of PNP was obtained within 6 min under optimized conditions. Moreover, the catalyst had a good stability and reusability, thus expanding the scope of non-iron based catalysts in the Fenton-like reactions.
研究领域:
环境化学
·
催化科学
·
环境污染与控制
·
高级氧化技术
·
材料化学
✓ 已验证
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2015
·
IF 3.453
Xiaoyun Chen,Dong-Hau Kuo,Dongfang Lu,Yongxuan Hou,Yen-Rong Kuo
Mesoporous TiO 2 was synthesized by a hydrolysis precipitation method with the utilization of the biological renewable resource of lignin as template and TiCl 4 as reactant. The photocatalytic activity of TiO 2 was investigated by the degradation of phenol under UV light irradiation. The microstructure, crystallinity , powder characteristic, and chemical bonding of the catalyst were analyzed. The 500 °C-calcined TiO 2 had average crystallite size of about 11.1 nm and a mesoporous structure with specific area of 165.8 m 2 /g and pore volume of 0.312 cm 3 /g. The results showed that TiO 2 synthesized with lignin template exhibited high photocatalytic activity, which can be attributed to the electronegativity and the network skeleton of lignin to uniformly distribute the TiO 2 precursor for forming TiO 2 mesoporous particles. The mechanism for the improved photodegradation of the lignin-assisted TiO 2 was proposed.
研究领域:
材料科学
·
环境化学
·
纳米技术
·
光催化
·
绿色化学
✓ 已验证
DOI
高影响因子
Royal Society Open Science
·
2018
·Vol. 5
·期 4
·
IF 2.504
Donglin He,Huiping Zhang,Ying Yan
Cu-ZSM-5 catalysts were prepared by chemical vapour deposition for catalytic wet peroxide oxidation (CWPO) of phenol in a fixed bed reactor. Firstly, Cu-ZSM-5 catalysts with Cu loading of 0.5, 2, and 6 wt% were prepared and characterized by X-ray diffraction (XRD), N2 adsorption–desorption and X-ray photoelectron spectra (XPS). The characterization results demonstrated that CuO was uniformly dispersed on ZSM-5 with slight effect on the structure properties of the support. Then, several variables, such as the copper loading, reaction temperature, catalyst bed height and feed flow rate were investigated in the CWPO of phenol in aqueous solution at high concentration (1000 ppm). Compared with the catalyst prepared by the impregnation method, the Cu-ZSM-5 prepared by chemical vapour deposition has a better capacity of further oxidizing the intermediate organic products into carbon dioxide and water with less metal loading. Based on the Cu-ZSM-5 catalyst with Cu loading of 6 wt%, complete removal of phenol and a high TOC reduction (around 70%) have been achieved at the temperature of 80°C feed flow rate of 2 ml min−1 and catalyst bed height of 3 cm. Moreover, this catalyst maintained high catalytic activity after three runs with high phenol conversion (94%) under this optimum operating condition. Finally, the reaction mechanism was studied based on the intermediates detected by high-performance liquid chromatography (HPLC).
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL ENGINEERING
·
2019
·Vol. 145
·期 12
·04019083
·
IF 1.657
Yuechao Zhang,Dian Yang,Ping Ning,Yingjie Li,Senlin Tian,Junjie Gu
The aim of this work was to study the supercritical water (SCW) regeneration of phenol-saturated activated carbon (AC) with the H2O2 and alkali metal catalyst (Na2CO3, NaOH, K2CO3, and KOH) addition. The results showed that SCW could effectively regenerate AC in the 385–425°C range without any additives, but large and small amounts of phenol and dibenzofuran were present in the liquid phase, respectively, which would result in secondary pollution. The H2O2 addition enhanced the decomposition of phenol and increased the CO2 yield. With the addition of H2O2 and an alkali metal catalyst, SCW further decreased the phenol and dibenzofuran yields but increased the H2 and CO2 yields. Active component-supported (Cu-Ce-O, Fe-Ce-O, Ni-Zn-Pt, and Ni-Co-Pt) AC adsorbents might have decomposed some of the phenol during the phenol adsorption process, which resulted in relatively small amounts of phenol adsorbed on the AC and a decrease of the liquid (phenol and dibenzofuran) and gaseous (H2 and CO2) yields. SCW regeneration increased the surface area and pore volume of the AC and raised the adsorption capacity. The H2O2 and alkali metal catalyst addition can be used to achieve the rapid, efficient, and harmless regeneration of AC in SCW at a lower temperature (385°C).
研究领域:
环境工程
·
化学工程
·
材料科学
·
污染控制
·
绿色化学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Lixi Yang,Defeng Yin,Yanxia Zheng,Yubo Yang,Yuchao Li,Jinguo Hao,Bing Ai,Tingting Ge,Cuncun Zuo,Xiaobin Wang,Qian Wang,Ming Wang,Haofei Huang
A series of cobalt-nitrogen modified catalysts were prepared and applied to the degradation of phenol . The Mott Schottky catalyst (CoO/NGr@C) with high pyridine nitrogen content was designed to activate potassium peroxodisulfate (PDS) to generate active free radicals for phenol degradation. The structural properties of the materials are analyzed by XPS , TEM and then the charge density calculation is performed by DFT, which proves the existence of the highly active interface effect. Co–N-C MCM-41 can only degrade phenol into benzoquinone and it is difficult to achieve further degradation of benzoquinone, while the modified CoO/NGr@C can achieve deep mineralization of the intermediate benzoquinone through UV spectrum. EPR was used to prove that both hydroxyl radicals and sulfate radicals exist in the degradation process of phenol. Through the DFT simulation calculation of the material, it is proved that the existence of carbon activated by nitrogen and the electron rearrangement between cobalt and nitrogen-rich carbon lead to the catalytic activity of the material. The degradation conditions of phenol were optimized and the reaction kinetics of further phenol degradation were studied. The activation energy of phenol degradation on CoO/NGr@C is calculated to be 34.38 kJ mol −1 .
研究领域:
环境化学
·
催化科学
·
材料科学
·
物理化学
·
环境污染治理
·
自由基反应机制
·
理论计算化学
✓ 已验证
DOI
高影响因子
WATER SCIENCE AND TECHNOLOGY
·
2021
·Vol. 84
·期 12
·3871-3890
·
IF 1.915
Liu Chenyu,Wei Haitong,Gao Yanhui,Wang Ning,Yuan Xiaoying,Chi Zhilong,Zhao Guangli,Song Shuguang,Song Jianjun,Jin Xinghui
Metal-organic frameworks (MOFs) have unique properties and stable structures, which have been widely used as templates/precursors to prepare well developed pore structure and high specific surface area materials. In this article, an innovative and facile method of crystal reorganization was designed by using MOFs as sacrificial templates to prepare a layered double hydroxide (LDH) nano-layer sheet structure through a pseudomorphic conversion process under alkaline conditions. The obtained CoMn-LDH and CoFe-LDH catalysts broke the ligand of MOFs and reorganized the structure on the basis of retaining a high specific surface area and a large number of pores, which had higher specific surface area and well developed pore structure compared with LDH catalysts prepared by traditional methods, and thus provide more active sites to activate peroxymonosulfate (PMS). Due to the unique framework structure of MOFs, the MOF-derived CoMn-LDH and CoFe-LDH catalysts could provide more active sites to activate PMS, and achieve a 2,4-dichlorophenol degradation of 99.3% and 99.2% within 20 minutes, respectively. In addition the two LDH catalysts displayed excellent degradation performance for bisphenol A, ciprofloxacin and 2,4-dichlorophenoxyacetic acid (2,4-D). X-ray photoelectron spectroscopy indicated that the valence state transformation of metal elements participated in PMS activation. Electron paramagnetic resonance manifested that sulfate radical ( ) and singlet oxygen ( 1 O 2 ) were the main species for degrading pollutants. In addition, after the three-cycle experiment, the CoMn-LDH and CoFe-LDH catalysts also showed long-term stability with a slight activity decrease in the third cycle. The phytotoxicity assessment determined by the germination of mung beans proved that PMS activation by MOF-derived LDH catalysts can basically eliminate the phytotoxicity of a 2,4-D solution. This research not only developed high-activity LDH catalysts for PMS activation, but also expanded the environmental applications of MOF derivants. LDH derived from MOFs through a pseudomorphic conversion process. LDH showed excellent activity to activate PMS to degrade 2,4-DCP and other pollutants. CoMn-LDH and CoFe-LDH exhibited high stability and reusability. High specific surface area and well developed pore structure of LDH provide more active sites. Phytotoxicity assessment displayed the practical application value of LDH.
研究领域:
环境化学
·
材料科学
·
催化化学
·
环境污染治理
·
纳米材料
·
自由基反应机制
·
可持续环境技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）