JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Keke Li,Sen Li,Wule Zhang,Zhifeng Shi,Di Wu,Xu Chen,Pei Lin,Yongtao Tian,Xinjian Li
Photocatalytic applications of halide perovskites have attracted increasing attention. However, lack of stability and lead toxicity of lead halide perovskites have hindered their applications. Metal halide double perovskite (DP) Cs 2 AgInCl 6 is a stable, environment-friendly semiconductor with direct band gap, and then the best promising alternative to lead halide perovskites. Here, the applications of Cs 2 AgInCl 6 DP to photocatalytic degradation of organic pollutants have been developed, in which the octahedral Cs 2 AgInCl 6 DP particles (~3.33 eV) were prepared by precipitation from acid solutions. The as-prepared samples exhibit high photocatalytic activity, which can degrade about 98.5% of water-insoluble carcinogen Sudan Red III in only 16 min, and have a good stability for 5 cycle operations. Furthermore, the Cs 2 AgInCl 6 DP also can degrade Rhodamine B, Methyl orange and Methyl red efficiently, demonstrating a highly-efficient and stable ethanol solvent-based photocatalytic system for organic pollutants degradation. The high photocatalytic activity could be attributed to direct band gap and long carrier lifetime of Cs 2 AgInCl 6 DP. These unique features of Cs 2 AgInCl 6 DP indicate that it could have a good application prospect for photocatalytic degradation of organic pollutants.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Ning Min,Jun Yao,Meseret Amde,Cengceng Tang,Langping Wu,Hans Hermann Richnow,Yafei Chen,Yongqiang Cui,Hao Li
Compound-specific isotope analysis (CSIA) is a useful technique that has received an increasing attention for studying the degradation mechanisms of organic contaminants based on stable isotope fractionation concepts. This study reports the degradation mechanisms of p -chloroaniline (PCA) at different pH values (3, 5, 7 and 9) induced by persulfate (PS) based on 13 C isotope fractionation during its preferential oxidation with SO 4 − and OH. The results showed that the degradation of PCA followed first-order kinetics (rate constants, 0.026, 0.0362, 0.0754 and 0.0497 h −1 at pH = 3, 5, 7 and 9, respectively), with the fastest degradation under neutral conditions (pH 7). The degradation rate was found to be higher under alkaline conditions (pH 9) compared to acidic conditions (pH 3 and 5). A normal carbon isotope fractionation of PAC was observed under neutral and alkaline conditions (eg., ε C = −0.8‰ ±0.10 at pH 7 and ε C = −1.0‰ ±0.17 at pH 9). However, a reverse carbon isotope effect at pH 3 (ε C = 0.6‰ ±0.07) and pH 5 (ε C = 1.1‰ ±0.06) was observed, respectively. Based on the identified transformation products and the insights revealed by CSIA, the degradation pathways were proposed. The current findings are crucial in understanding the PCA degradation mechanisms with SO 4 − and OH in aqueous systems.
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Nature Sustainability
·
2021
·Vol. 4
·期 7
·618-626
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IF 19.346
Chen Yao,Xu Mengjiao,Wen Jieya,Wan Yu,Zhao Qingfei,Cao Xia,Ding Yong,Wang Zhong Lin,Li Hexing,Bian Zhenfeng
Precious metals such as gold and platinum are valued materials for a variety of important applications, but their scarcity poses a risk of supply disruption. Recycling precious metals from waste provides a promising solution; however, conventional metallurgical methods bear high environmental costs and energy consumption. Here, we report a photocatalytic process that enables one to selectively retrieve seven precious metals—silver (Ag), gold (Au), palladium (Pd), platinum (Pt), rhodium (Rh), ruthenium (Ru) and iridium (Ir)—from waste circuit boards, ternary automotive catalysts and ores. The whole process does not involve strong acids or bases or toxic cyanide, but needs only light and photocatalysts such as titanium dioxide (TiO 2 ). More than 99% of the targeted elements in the waste sources can be dissolved and the precious metals recovered after a simple reducing reaction that shows a high purity (≥98%). By demonstrating success at the kilogram scale and showing that the catalysts can be reused more than 100 times, we suggest that this approach might be industry compatible. This research opens up a new path in the development of sustainable technologies for recycling the Earth’s resources and contributing to a circular economy.
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CHEMICAL ENGINEERING JOURNAL
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2021
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IF 13.273
Zhuo-Yu Li,Yu-Lei Liu,Pei-Nan He,Xin Zhang,Lu Wang,Hai-Teng Gu,Hao-Chen Zhang,Jun Ma
Hydroxylamine is commonly known to enhance the performance of Fe(II)-based advanced oxidation processes (AOPs) by promoting Fe(II) regeneration from Fe(III). Recently, ferryl ion (Fe(IV)) was found as an important reactive specie in Fe(II)/peroxydisulfate (PDS) system, while the interaction between hydroxylamine and Fe(IV) in Fe(II)/hydroxylamine/PDS system was still ambiguous. Therefore, the role of hydroxylamine, especially in interaction with reactive species, was systematically studied therein. With methyl phenyl sulfoxide (PMSO) as a probe compound, an original function of hydroxylamine to transform the major reactive species from Fe(IV) to radicals (SO 4 - and OH) for potential pollutants oxidation was clarified. Experimental results combined with Density Functional Theory (DFT) calculations showed that SO 4 - , OH and Fe(IV) all contributed to PMSO oxidation. Hydroxylamine showed the greatest promotional effect on the production of SO 4 - , while the production of Fe(IV) was inhibited with concentrations of hydroxylamine increasing from 0.2 to 1.4 mM. Compared with PMSO, hydroxylamine showed stronger scavenging ability towards Fe(IV) than SO 4 - and OH. Thus, more than 50% of radicals was consumed by PMSO and Fe(IV) mainly reacted with hydroxylamine to regenerate Fe(II). In a word, hydroxylamine played a dual role during potential pollutants oxidation in Fe(II)/hydroxylamine/PDS system, namely (1) transforming the major reactive species from Fe(IV) to radials (SO 4 - and OH) and (2) regenerating Fe(II) from both Fe(IV) and Fe(III). This study provides an insight into the role of hydroxylamine and its interactions with Fe(IV), which advances our understanding on similar Fe(II)/reductants/PDS systems.
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Surfaces and Interfaces
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2021
·
IF 4.837
Chunli Wang,Yunxiang Dai,Xiaoheng Fu,Hongbo Lu,Jing Zhang
In this work, a novel 2-dimentional (2D)-2D bentonite/g-C 3 N 4 composite (B/g-C 3 N 4 ), with a layer-layer cross structure and large surface area, was synthesized by a self-assembly process, with the aim for the photocatalytic oxidation of arsenic (As(III)) in wastewater. The structure and properties of the mineral-based composite were characterized by X-ray diffraction (XRD), infrared spectroscopy (IR), scanning electron microscopy (SEM), and photocurrent measurements. The photocatalytic activity of 2D-2D B/g-C3N4 for As(III) removal was further investigated under visible light . The results reveal that the As(III) oxidation rate by 2D-2D B/g-C3N4 composite was three times higher than that by pure g-C3N4, owing to the enlarged specific surface area and the suppressed electron–hole recombination by the incorporated bentonite. Moreover, the composite exhibited a high photocatalytic oxidation efficiency in a wide pH adaptability from 3 to 8.5. Through electron spin resonance (ESR) technique and radical quenching experiments, the photocatalytic mechanism of As(III) oxidation was proposed, where superoxide radicals played a critical role in the photo-oxidation of As(III) in both acid and basic conditions. This work paved a new way to design the mineral-based photocatalyst for treatment of pollutants in a wide pH range.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Chang-Long Tan,Ming-Yu Qi,Zi-Rong Tang,Yi-Jun Xu
Highly efficient photodriven conversion from biomass-derived platform chemicals to value-added chemical feedstocks and clean fuel hydrogen (H 2 ) possesses immense potential to cope with the existing energy and environmental problems. We herein report a facile approach combining hydrothermal method and photodeposition method for fabricating diverse sulfide-based cocatalysts (MoS 2 , NiS and WS 2 ) decorated ZnIn 2 S 4 (ZIS) for simultaneous exploitation of photogenerated electrons and holes, effectively achieving the oxidation of furfuryl alcohol (FOL) cooperative with H 2 evolution in one photoredox cycle. The results show the optimal binary MoS 2 -ZIS composites can obtain almost 7 times yield of products (furfural and H 2 ) as high as that of blank ZIS. Notably, compared with previous reports in literatures, our present MoS 2 -ZIS shows the best performance in this photoredox dual reaction. As a relay station for electrons, cocatalysts facilitate the separation and transfer of photogenerated charge carriers in the composites, therefore prominently improving the photocatalytic performance. We anticipate that the present work can offer insights to guide the design of photoredox reaction systems for efficient valorization of biomass-derived platform chemicals.
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CARBON
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2021
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IF 9.594
Xiaocui Wu,Qingshan Zhao,Fang Guo,Guangsen Xia,Xiaojie Tan,Huiyuan Lv,Zhaoxuan Feng,Wenting Wu,Jingtang Zheng,Mingbo Wu
Merging photocatalysis with Fenton-like reaction provides a promising synergetic advanced oxidation technology for water treatment, whereas the rational design of efficient cooperative photo-Fenton system still remains a great challenge. In this study, a ternary α-FeOOH/carbon dots/porous g-C 3 N 4 (α-FeOOH/CDs/p-GCN) composite is developed as visible-light-driven heterogeneous photo-Fenton catalyst for contaminated water remediation. α-FeOOH nanorods are in-situ grown on porous g-C 3 N 4 substrates, among which CDs are intercalated as high-speed electron transmission bridges, simultaneously preventing the photogenerated electron-hole recombination and accelerating the Fe 3+ /Fe 2+ redox cycle. The distinctive heterostructure and synergetic catalytic effect endow α-FeOOH/CDs/p-GCN with superior efficiency, reusability , and universality for recalcitrant pollutant elimination, the reaction rate of which is nearly 13.6, 7.3, 3.4, 1.4, and 5.1 times higher than that of α-FeOOH, bulk g-C 3 N 4 (b-GCN), p-GCN, α-FeOOH/p-GCN, and α-FeOOH/CDs/b-GCN, respectively. The FeOOH/CDs/p-GCN also demonstrates excellent tolerance to realistic environmental matrices including deionized water, sea water, river water, wastewater, and underground water. HO• and •O 2 − radicals are proved to be the predominant contributors in the photo-Fenton system. This work provides an efficient synergetic visible-light-driven photo-Fenton catalyst possessing great potential for practical contaminated water remediation.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
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IF 9.028
Wei Wu,Shishu Zhu,Xiaochen Huang,Wei Wei,Chao Jin,Bing-Jie Ni
Persulfate (PS) activation on biochar (BC) is a promising technology for degrading the aqueous organic contaminants. However, the complexity of activation mechanisms and components in biomass that used to produce BC makes it difficult to predict the performance of PS activation. In this study, we employed eight sludges as the representative biomass that contained absolutely different organic or inorganic components. Results showed that the elemental composition, surface properties, and structures of the sludge-derived BCs (SBCs) clearly depended on the inherent components in the sludges. The intensities of persistent free radicals (PFRs) in the electron paramagnetic resonance (EPR) correlated positively with N-containing content of sludges as electron shuttle, but negatively with the metal content as electron acceptor. Linking with PFRs as crucial sites of triggering a radical reaction, a poly-parameter relationship of predicting PS activation for organic degradation using the sludge components was established (kobs,PN = 0.004 × Cprotein + 0.16 × CM–0.895 −0.118). However, for the PS activation on those SBCs without PFRs, this redox process only relied on the sorption or conductivity-related characteristics, not correlating with the content of intrinsic components in biomass but with pyrolysis temperatures. This study provided insightful information of predicting the remediation efficiency of PS activation on BCs and further understanding the fate of contaminants and stoichiometric efficiency of oxidants in a field application.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Haocheng Song,Qiang Li,Yuxuan Ye,Fei Pan,Dajie Zhang,Dongsheng Xia
Antibiotic contamination has become a serious environmental problem and much attention has been paid to its purification. The sulfate radical (SO 4 − ) based advanced oxidation processes (AOPs) exhibited significant potential in the treatment of antibiotics. In this study, the magnetic biochar (Fe 2 O 3 @LBC) derived from loofah was prepared to activate persulfate (PS) for cephalexin (CEX) degradation. Under the optimal conditions, 73.9% of CEX was removed in the Fe 2 O 3 @LBC/PS system. Free radicals quenching experiments and electron paramagnetic resonance (EPR) analysis revealed that HO and SO 4 − were responsible for the degradation of CEX. The C-OH of the catalyst played a crucial role in the degradation process. In addition, the conversion between Fe 3+ and Fe 2+ enhanced the degradation of CEX by producing SO 4 − . The degradation performance of other antibiotics and CEX in different water matrices indicated the broad adaptability and applications of Fe 2 O 3 @LBC. The main intermediates and the possible transformation pathways were proposed. These results provided a potential insight into biochar based catalysts for the degradation of antibiotics by activation of persulfate.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
·
IF 10.588
Yunjin Yao,Huanhuan Hu,Hongda Zheng,Hongwei Hu,Yinghao Tang,Xiaoyan Liu,Shaobin Wang
Bimetallic Fe- and Mo-embedded N-enriched porous biochar (Fe-Mo@N-BC) is developed and serves as a cost-effective and highly efficient catalyst for mineralization of non-biodegradation organic contaminants . Fe-Mo@N-BC was prepared by pyrolysis of complex Fe/Mo -containing precursors. Transmission electron microscopy and elemental mapping suggested that Fe and Mo are uniformly dispersed in nitrogen-doped biochar with hierarchical mesopores . In comparison to Fe@N-BC and Mo@N-BC, Fe-Mo@N-BC exhibited a superior activity for activating peroxymonosulfate (PMS). The stable activity was ascribed to N-doping and synergistic effect of Fe and Mo species, where both Fe-N x and Mo-N x can simultaneously serve as the active sites and N-BC can act as a carrier and an activator as well as an electron mediator. Electron paramagnetic resonance and quenching experiments indicated that H O • , O 2 • − and 1 O 2 were responsible for organic degradation . The effects of PMS dosage, initial Orange II concentration, temperature, solution pH, coexisting anions and humic acids on organic degradation were also investigated. With the assistance of an external magnet, Fe-Mo@N-BC can be easily separated after reaction and remains stable in the reusability tests. This work demonstrates a feasible strategy towards the fabrication of Fe, Mo-embedded N-enriched porous biochar catalysts for the detoxification of organic contaminants.
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CHEMOSPHERE
·
2021
·
IF 7.086
Ji'an Sun,Lixin Wang,Yuge Wang,Weiyang Lv,Yuyuan Yao
The morphology and specific surface area of layered double hydroxide (LDH) are of great significance for optimizing the application of LDH in sewage treatment . Herein, we present a study of the relation between the catalytic property and the morphology of LDH via activating peroxymonosulfate (PMS) for degradation of organic pollutants. The results demonstrated that LDH nanoscrolls possessed a superior performance for methylene blue (MB) degradation, which achieved almost 100% removal in 40 min and the calculated apparent rate constant was about 2.1, 4.5 and 11.5 times higher than that of LDH nanosheets, Co 2+ and Co 3 O 4 , respectively. According to the results of X-ray photoelectrons spectroscopy (XPS) and electron paramagnetic resonance (EPR), 1 O 2 was confirmed to play a dominant role in the MB degradation, where the redox cycle of Co 3+ /Co 2+ provided the impetus for the reaction. Moreover, the pH and ion tolerance abilities of LDH nanoscrolls in PMS activating process were determined as well. Remarkably, CO 3 2− and H 2 PO 4 − could even promote the generation of •OH and 1 O 2 to facilitate the progress of reaction. Overall, these findings in the study may provide more opportunities in the preparation of high-efficiency catalysts and give insight into the accelerated degradation of refractory contaminants with surrounding anions.
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ACS ES&T Engineering
·
2021
·
IF 0
Cong Wang,Shao-Yi Jia,You Han,Yang Li,Yong Liu,Hai-Tao Ren,Song-Hai Wu,Xu Han
Enzymatic polymerization of phenolic contaminants to polyphenolics by H2O2 is an effective method to turn phenolic wastes to useful polymers. However, the sensitivities and the high costs of enzymes always limit their applications in the long-run treatment of industrial wastewater. In this study, a highly efficient CuO-persulfate (PS) system is reported to be a promising candidate for enzyme–H2O2 and shows high reactivity to polymerize various phenolic contaminants to polymers under alkaline conditions with the ratio of PS/phenolics less than 2.0. Compared with the generally accepted mechanism that the oxidizing species of SO4•– and ·OH generated during PS activation primarily contribute to the oxidation of various organic contaminants, quenching experiments, EPR (electron paramagnetic resonance) analysis and DFT calculations in this study indicate that PS is activated on CuO via a nonradical pathway under alkaline conditions, and the O–O bond in PS is moderately elongated from 1.45 to 1.58 Å. The inversely linear relationship between log kobs and BDEO–H values of various phenolics in the Hammett plot confirms H-abstraction from various phenolics under alkaline conditions. DFT calculations further reveal the formation of phenolic radicals after the activated PS abstracts H from phenolic −OH, followed by subsequent polymerization of phenoxyl radicals to polyphenolics. Characterizations of the oxidation products confirm that more than 80% phenolic contaminants have been transformed to polyphenolics. This study provides a new alternative for recovering various phenolic contaminants from industrial wastewater.
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