APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Chuanqiang Li,Xiang Liu,Tao Peng,Tong Zhang,Chuanchuan Lin,Yangyang Zhang,Qianqian Chai,Wenge Qiu,Liyun Song
A Co/Mn-based metal – organic framework was used as a precursor to synthesize oxygen-rich defects in binary Co – Mn oxides using mechanical-coordination chemistry method. The samples were characterized using X-ray diffraction, Raman spectroscopy, N 2 adsorption–desorption analysis, scanning-electron microscopy, X-ray photoelectron spectroscopy, electron paramagnetic resonance, and transmission-electron microscopy. H 2 -temperature-programmed reduction and O 2 -temperature-programmed desorption analyses were performed to examine the redox properties and mobility of the oxygen species in the catalysts, respectively. The sample obtained from Co/Mn-BTC-2/3 exhibited the highest catalytic activity for the total oxidation of propane, with a T 90 of 255 ℃ at 120 L g −1 h −1 . The considerable performance of the sample is associated with its smaller grain size , larger specific surface area, and abundant interface and oxygen defects. This study offers a simple strategy for the synthesis of Co/Mn-BTC with hexanuclear SBUs, further deriving to oxygen-deficient and high-performance propane elimination catalysts, which could potentially be applied on an industrial scale.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Kexin Yin,Yanan Shang,Dongdong Chen,Baoyu Gao,Qinyan Yue,Xing Xu
Versatile persulfate-based catalytic mechanisms induced by highly-effective single atom catalysts (SACs) have been intensively reported, which was mainly ascribed to the versatile coordinated-structures of SACs. However, the origin of these different mechanisms from the specific properties of pollutants has been ignored. In this work, eight kinds of pollutants were selected and the half-wave potential (φ 1/2 ) values representing their redox potentials were determined. A good correlation between the redox potential characteristics of pollutants and their oxidation performances/pathways in manganese single-atom catalyst (Mn-SAC)/PMS system can be confirmed. The φ 1/2 values of different pollutants showed a good correlation with the energy gaps between the pollutants and Mn-SAC/PMS complexes as well as their electrophilicity indexes, which confirmed the redox potential of pollutants was essential to the electron-transfer oxidation in Mn-SAC/PMS system. Based on the new insights in this work, we will be able to unveil the sources of Fenton-like systems with tunable oxidation processes.
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Nanomaterials
·
2022
·Vol. 12
·期 22
·3994
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IF 5.719
Zhanwu Wang,Yingrui Sui,Meiling Ma,Tianyue Wang
Cu2ZnSn(S,Se)4(CZTSSe) films are considered to be promising materials in the advancement of thin-film solar cells. In such films, the amounts of S and Se control the bandgap. Therefore, it is crucial to control the concentration of S/Se to improve efficiency. In this study, Cu2MnxZn1−xSnS4(CMZTS) films were fabricated using the sol-gel method and treated in a Se environment. The films were post-annealed in a Se atmosphere at various temperature ranges from 300 °C to 550 °C at intervals of 200 °C for 15 min to obtain Cu2MnxZn1−xSn(S,Se)4(CMZTSSe). The elemental properties, surface morphology, and electro-optical properties of the CMZTSSe films were investigated in detail. The bandgap of the CMZTSSe films was adjustable in the scope of 1.11–1.22 eV. The structural propeties and phase purity of the CMZTSSe films were analyzed by X-ray diffraction and Raman analysis. High-quality CMZTSSe films with large grains could be acquired by suitably changing the selenization temperature. Under the optimized selenization conditions, the efficiency of the fabricated CMZTSSe device reached 3.08%.Keywords:Cu2ZnSn(S,Se)4film;Mn-doping;solar cells;properties;selenization temperature
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International Journal of Chemical Reactor Engineering
·
2022
·Vol. 21
·期 5
·663-678
·
IF 1.636
Feng Guo,Hua-jie Liu,Xin-zhi Zhou,Xiang-li Long
In this paper, a heterogeneous catalytic system consisting of Co/Mn/Br/activated carbon is used to catalyze 2-nitro-4-methylsulfonyl benzoic acid (NMSBA) production from the oxidation of 2-nitro-4-methylsulfonyltoluene (NMST) by oxygen. The activated carbon (AC) is made from coconut shell with acetic acid as an activator. The experiments indicate that the best AC is made by immersing coconut shell in 12 mol L −1 HAc solution at 50 °C for 32 h with a liquid/solid ratio (mL/g) of 5:1 and then being heated in nitrogen at 800 °C for 6 h. Compared with the Co/Mn/Br/H 3 PMo 12 O 40 @CAC (CAC, commercial activated carbon originated from coconut shell) catalytic system, the Co/Mn/Br/AC catalytic system is able to gain much higher NMSBA selectivity. In spite of holding smaller surface and less acidic groups, the AC owns much more carboxyl than CAC, which is the main reason for its better performance in the preparation of NMSBA.
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JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Jun Luo,Xiaofang Ruan,Wuying Chen,Sha Chen,Zhexu Ding,Ang Chen,Ding Li
Recently, biogenic Mn oxides (BioMnO x ) are considered as the promising degradation agents for environmental organic contaminants . However, little information is available for the degradation of atrazine by BioMnO x . In this work, BioMnO x , generated by a soil-derived Mn(II)-oxidizing bacterium, Providencia sp. LLDRA6, was explored to degrade atrazine. To begin with, collective results from mineral characterization analyses demonstrated that this BioMnO x was biogenic bixbyite-type Mn 2 O 3 . After that, purified biogenic Mn 2 O 3 was found to exhibit a much higher removal efficiency for atrazine in aqueous phase, as compared to unpurified biogenic Mn 2 O 3 and LLDRA6 biomass. During the atrazine removal by biogenic Mn 2 O 3 , six intermediate degradation products were discovered, comprising deethylatrazine (DEA), hydroxylatrazine (HA), deethylhydroxyatrazine (DEHA), ammeline, cyanuric acid , and 5-methylhexahydro-1,3,5-triazine-2-thione (MTT). Particularly, the intermediate, MTT, was considered as a new degradation product of atrazine, which was not described previously. Meanwhile, Mn(II) ions were released from biogenic Mn 2 O 3 , and on the surface of biogenic Mn 2 O 3 , the content of hydroxyl O species increased at the expense of that of lattice and water O species, but the fundamental crystalline structure of this Mn oxide remained unchanged. Additionally, no dissociative Mn(III) was found to involve in atrazine degradation. In summary, these results demonstrated that both the non-oxidative and oxidative reactions underlay the degradation of atrazine by biogenic Mn 2 O 3 .
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Qiuli Fu,Ximeng Xu,Rongrong Miao,Minli Wang,Huajing Zhou,Liang He,Qingqing Guan
Using some metals and their oxides modified biochar adsorbents to purify copper-containing wastewater is effective. However, the degraded reuse performance of waste adsorbents prevented their large-scale application. Thus, in this work, a MnO x -modified porous biochar was firstly obtained by KMnO 4 activation of rubber seed shell wastes for Cu(II) ions removal, and then the waste adsorbent was skillfully constructed to Cu-Mn bimetallic catalyst for efficient selective hydrogenation of furfural, realizing the proper disposal of waste adsorbent. The adsorption experiments showed that the optimized Mn-modified biochar (i.e. Mn 18% - rss BC) had a good purification capacity for the Cu(II)-containing wastewater with a wide pH range and high strong resistance to some common coexisting ions, and the maximum adsorption capacity of Cu(II) could be up to 200.59 mg/g. The characterization results showed that the oxygen-containing functional groups and a large number of MnO x particles on the surface of Mn 18% - rss BC could form stable complexes with Cu(II), making it exhibit efficient and spontaneous multilayer adsorption behavior. In addition, after the reduction of the waste adsorbent, the Cu and Mn species on the surface were uniformly dispersed in the porous carbon in the form of electron-rich nano-polycrystalline aggregates at about 3.5 nm. Under the optimized conditions, the obtained catalyst (i.e., Cu 14.3 Mn 16.5 - rss BC) had high catalytic efficiency, which can achieve 100% of furfural conversion and 87.06% of furfuryl alcohol selectivity. In conclusion, this work provided a composite solution for the reuse of copper-containing waste adsorbent, the resource recovery of agricultural and forestry wastes and the efficient transformation of biomass platform compounds.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Ma Bai,Youzheng Chai,Anwei Chen,Jihai Shao,Shiye Zhu,Jiayi Yuan,Zhenghang Yang,Jiahao Xiong,Doudou Jin,Keqi Zhao,Yanziyun Chen
The extensive utilization of neonicotinoid insecticides (NNIs) in agricultural practices ultimately poses a significant threat to both the environment and human health. This work focuses on the efficient degradation and detoxification of the representative NNI, thiamethoxam (THX), and explores the underlying mechanism using a Co-Fe-Mn mixed spinel doped carbon composite catalyst activated persulfate. The findings demonstrate that the composite effectively degrades THX, achieving a degradation rate of 95% in 30 mins, while requiring only a fraction (one-sixteenth) of the oxidant dosage compared to pure carbon. The study aimed to examine the negative impact of reactive halogens on reactive oxygen species within a saline environment. The degradation byproducts were linked to the presence of two common electron-withdrawing groups, namely halogens and nitro in the THX molecule. It was hypothesized that the degradation process was primarily influenced by C-N bond breaking and hydroxylation occurring between the diazine oxide and 2-chlorothiazole rings. Consequently, dehalogenation and carbonylation processes facilitated the elimination of halogenated components and pharmacophores from the THX, leading to detoxification. In addition to the identified free radical pathway including SO 4 • − , •OH and O 2 • − contributed to THX degradation, the participation of non-radical pathways ( 1 O 2 and electron transfer) were also confirmed. The efficacy of detoxification was further validated through toxicity assessment, employing quantitative conformation relationship prediction and microbial culture utilizing Bacillus subtilis .
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RSC Advances
·
2020
·Vol. 10
·期 53
·32249-32258
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IF 3.119
Fengli Liu,Huosheng Li,Dandan Liao,Yanhong Xu,Mingxia Yu,Shengwen Deng,Gaosheng Zhang,Tangfu Xiao,Jianyou Long,Hongguo Zhang,Yuting Li,Keke Li,Ping Zhang
Carbon quantum dots (CQDs) were synthesized via a hydrothermal method, in which extracellular polymeric substance (EPS) from anaerobic ammonium oxidation (anammox) granular sludge was used as a carbon precursor, while citric acid and ethylenediamine were applied as auxiliary carbon source and passivation agent, respectively. The synthesized CQDs, with orderly spherical shape and mean size of 7.15 nm, emitted blue fluorescent light under UV radiation of 365 nm. The CQDs had a high fluorescence yield (40.84%), with good water solubility and excellent spectroscopic properties. In addition, the CQDs exhibited selective, sensitive and distinctive fluorescence quenching behaviors for Cr(VI) and Mn(VII) in a PBS buffer solution (NaH2PO4–Na2HPO4) of pH 7, with a detection limit of 5.8 nM for Cr(VI) and 2.3 nM for Mn(VII). Owing to the nitrogen components from the EPS of anammox granules, the CQDs were well nitrogen-doped, promoting electron-transfer and leading to reduction between the CQDs and Mn(VII)/Cr(VI). These results indicate that CQD-based chemical sensing is a simple and efficient means for the fluorescence detection of Mn(VII) and Cr(VI).
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2021
·
IF 6.064
Bichun Huang,Hansun Fang,Huajun Huang,Meijuan Lu,Chenglong Yu
A one-pot synthetic method was used to prepare copper (Cu)-modified manganese (Mn)-rich MnSAPO-34 catalysts, which were then used for NO x removal from stationary-source flue gas. The addition of Cu to these Mn-rich MnSAPO-34 catalysts significantly enhanced their low temperature (LT) selective catalytic reduction (SCR) activity and H 2 O resistance. The Mn 0.4 Cu 0.05 SAPO-34 catalysts demonstrated excellent LT NH 3 -SCR activity, with NO x removal being >90% from 160 to 300 °C. In addition, Mn 0.4 Cu 0.05 SAPO-34 catalysts exhibited high H 2 O resistance. This excellent performance was ascribed to strong synergistic effects between Mn 4+ and isolated Cu 2+ species in Mn 0.4 Cu 0.05 SAPO-34 catalysts, leading to suitable redox ability. The results of in situ FT-IR analysis indicated that LT-SCR reactions mainly proceeded by an Eley–Rideal reaction pathway at 200 °C in Cu-modified manganese-rich MnSAPO-34 catalysts. Thus, Mn 0.4 Cu 0.05 SAPO-34 was considered as a promising candidate for NO x removal from flue gas of stationary sources at low temperatures.
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ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Junhua Li,Lingzhi He,Jianbo Jiang,Zhifeng Xu,Mengqin Liu,Xing Liu,Haixia Tong,Zeng Liu,Dong Qian
In this work, three kinds of bimetallic Prussian blue analogues (PBAs), i.e. K x Ni [Fe(CN) 6 ]·nH 2 O (NiFe-PBA), K x Co [Fe(CN) 6 ]·nH 2 O (CoFe-PBA), and K x Mn [Fe(CN) 6 ]·nH 2 O (MnFe-PBA), were synthesized by a simple precipitation method under identical conditions. Their chemical compositions , structures, morphologies, valences of transition metals, and electrochemical sensing performances for 2-nitrophenol (2-NP) are examined in details. It is found that all the prepared PBAs hold face-centered-cubic structures with near perfect cube morphologies for NiFe-PBA and CoFe-PBA and truncated cube morphology for MnFe-PBA. For the electrochemical detection of 2-NP, a wide detection range of 1.0–700.0 μM was obtained at all PBAs modified electrodes together with the sensitivities of 443.3, 368.0, and 339.0 μA cm −2 mM −1 and detection limits of 0.28, 0.46, and 0.59 μM achieved at NiFe-PBA, CoFe-PBA, and MnFe-PBA modified electrodes, respectively. The superiority in electrochemical sensing performance of NiFe-PBA to CoFe-PBA and MnFe-PBA may stem from its higher conductivity, lager electroactive surface area, and better intrinsic catalytic property of the transition metal in its framework. Furthermore, the constructed NiFe-PBA-based sensor displays good repeatability, long-term stability, and high selectivity together with desirable recoveries (97.8–103.9%) for the assay of 2-NP in water samples. The present work is the first report on the PBAs-based electrochemical sensors for 2-NP detection, which may promise a future of PBAs or PBAs-based materials for sensing applications.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Xiaofeng Wang,Zhe Zhao,Yang Xu,Qingbo Li
A series of 3DOM-Mn x Ce y Ti z catalysts with three-dimensionally ordered macroporous (3DOM) structure were synthesized by a soft template method. The high SCR activity of the 3DOM-Mn 3 Ce 1 catalyst at low temperature was owing to the excellent redox ability and rich Lewis and Brønsted acid sites of the catalysts, which were beneficial to improve the catalytic activity. However, the strong oxidizability of MnO x resulted in the nonselective oxidation of NH 3 and generation of N 2 O, decreasing the N 2 selectivity. After addition of Ti, the redox capacity of the 3DOM-Mn 3 Ce 1 Ti 1 catalyst decreased, and the NH 3 were strongly adsorbed on the acid sites, which enhanced the N 2 selectivity with a broadened temperature window of 240–440 °C and a high GHSV of 120000 h −1 . Furthermore, both the 3DOM-Mn 3 Ce 1 and 3DOM-Mn 3 Ce 1 Ti 1 catalysts showed remarkable tolerance of H 2 O. Finally, through in situ DRIFT analysis, the Langmuir-Hinshelwood (L-H) mechanism was confirmed as the dominant reaction pathway over the 3DOM-Mn 3 Ce 1 Ti 1 catalyst.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Guiyuan Cai,Yu Tian,Daikun Li,Jun Zhang,Lipin Li,Qinyu Wang,Huihang Sun,Haoran Zhang,Pu Wang
Here, we prepared a novel nanostructured Fe–Cu–Mn composite oxide (FCMO x ) adsorbent using an ultrasonic coprecipitation method. The maximum adsorption capacity of As(III) and As(V) reached 158.5 and 115.2 mg/g under neutral conditions, respectively. The effects of several environmental factors (coexisting ions, solution pH, etc.) on the removal of inorganic arsenic using FCMO x were studied through batch experiments. The results showed that except for PO 4 3– and high initial pH, it was not significantly affected by ionic strength and other existing anions, implying a higher selectivity and adaptability. Combined with EPR, FTIR, and XPS analysis, we concluded that the Cu component and the reactive oxygen species (ROS) it generates played a decisive role in maintaining the stability of the redox cycle between Mn(IV)/Mn(III)/Mn(II) and enhancing the oxidation efficiency of As(III). Meanwhile, the adsorption mechanism of As(V) was mainly through the replacement of the FCMO x surface –OH to form stable inner-sphere arsenic complexes, while the removal mechanism of As(III) may involve the process of synergistic oxidation and chemisorption coupling. Additionally, the effective removal of As from the simulated As-contaminated water and its satisfactory reuse performance make FCMO x adsorbents favorable candidates for the removal of As-contaminated water in the future.
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