Catalysts
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2023
·Vol. 13
·期 3
·529
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IF 3.9
Linshuang Xue,Chenyi Yuan,Shipeng Wu,Zhen Huang,Zhen Yan,Stéphane Streiff,Hualong Xu,Wei Shen
Coalbed methane is a significant source of methane in the atmosphere, which is a potent greenhouse gas with a considerable contribution to global warming, thus it is of great importance to remove methane in coalbed gas before the emission. Exploring the economical non-noble metal catalysts for catalytic methane combustion (CMC) has been a wide concern to mitigate the greenhouse effect caused by the emitted low-concentration methane. Herein, a series of Mn-doped Co3O4catalysts have been synthesized by the environmentally friendly solid-state method. As a result, the Mn0.05Co1catalyst performed the best CMC activity (T90= 370 °C) and good moisture tolerance (3 vol% steam). The introduction of an appropriate amount of manganese conduced Co3O4lattice distortion and transformed Co3+to Co2+, thus producing more active oxygen vacancies. Mn0.05Co1exhibited better reducibility and oxygen mobility. In situ studies revealed that methane was adsorbed and oxidized much easier on Mn0.05Co1, which is the crucial reason for its superior catalytic performance.Keywords:active oxygen;catalytic combustion;low-concentration;methane;Mn-Co3O4;solid-state
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Bioactive Materials
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2023
·
IF 18.9
Qiongyu Qin,Ming Yang,Yu Shi,Haijing Cui,Chunshu Pan,Wenzhi Ren,Aiguo Wu,Jianqing Hu
Currently, precise ablation of tumors without damaging the surrounding normal tissue is still an urgent problem for clinical microwave therapy of liver cancer. Herein, we synthesized Mn-doped Ti MOFs (Mn–Ti MOFs) nanosheets by in-situ doping method and applied them for microwave therapy. Infrared thermal imaging results indicate Mn–Ti MOFs can rapidly increase the temperature of normal saline, attributing to the porous structure improving microwave-induced ion collision frequency. Moreover, Mn–Ti MOFs show higher 1 O 2 output than Ti MOFs under 2 W of low-power microwave irradiation due to the narrower band-gap after Mn doping. At the same time, Mn endows the MOFs with a desirable T 1 contrast of magnetic resonance imaging (r 2 /r 1 = 2.315). Further, results on HepG2 tumor-bearing mice prove that microwave-triggered Mn–Ti MOFs nearly eradicate the tumors after 14 days of treatment. Our study offers a promising sensitizer for synergistic microwave thermal and microwave dynamic therapy of liver cancer.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Ao Zhang,Zhongqing Jiang,Shaoda Zhang,Penghua Lan,Naihua Miao,Weiheng Chen,Ning Huang,Xiaoning Tian,Yangjie Liu,Zhongyu Cai
We report the development of non-noble transition metal sulfide catalysts Mn-CuS-x for high-efficiency and selective H 2 O 2 production. In this study, we synthesized Mn-CuS-x with coral-shaped hierarchical porous structure through one-pot hydrothermal reaction. The Mn-CuS-x possesses large specific surface area with plenty of crystalline defects via heteroatom doping of Mn. The Mn-CuS-x kinetically favored 2e − pathway over 4e − pathway, resulting in high selectivity (>92%) to H 2 O 2 production and high H 2 O 2 concentration (∼24.5 mM at 0.6 V vs. RHE) within 3 h for the optimized Mn-CuS-2 catalysts (synthesized with a molar ratio of 1:3:8 (MnCl 2 ·4 H 2 O: CuCl 2 ·2 H 2 O: C 2 H 5 NS)). The Mn-CuS-2 showed excellent stability, indicating that the Mn-CuS electrocatalysts can simultaneously achieve both high stability and enhanced H 2 O 2 production. Our first-principles calculations further confirmed that the heteroatom Mn doping to CuS thermodynamically makes the 2e – -ORR pathway more favorable. This study provides a green, low-cost, and efficient route to produce H 2 O 2 , which is very promising for generating chemicals and liquid fuels.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Bing Li,Fulin Deng,Zheyu Li,Hao Xiong,Shuqu Zhang,Weili Dai,Jie Zhang,Lixia Yang,Jianping Zou,Xubiao Luo
Perovskite oxide, as a promising candidate for volatile organic compounds combustion, is incapable in practical application at present due to its low intrinsic activity resulting from inadequate active oxygen species. However, balancing the concentration of active oxygen species and robust structure for perovskite oxide is still challenging. Herein, an efficient perovskite-based catalyst (denoted as TA-La 0.9 Ag 0.1 MnO 3 ) was constructed through Ag substitution and subsequently tartaric acid etching of LaMnO 3 , which exhibits robustly boosted catalytic performance for toluene combustion compared with pristine LaMnO 3 , causing a ∼100 °C lower T 90 . In this study, Ag substitution could weaken the La-O hybridization, which effectively facilitates La cations removal by subsequent acid etching, thus sufficiently exposing active Ag and Mn species and generating more surface lattice oxygen, but also constructs Ag-Mn-O bridges within the matrix of Ag substituted LaMnO 3 . Acid etching enables the activation of Ag-O-Mn bridges with strong electron transfer ability from O to Ag atom, promoting the mobility of lattice oxygen, and consequently the low-temperature oxidation ability. Additionally, the exposed Ag and Mn as Lewis acid sites can effectively improve the adsorption capacity toward toluene molecules, which synergistically facilitates the toluene abatement. Notably, TA-La 0.9 Ag 0.1 MnO 3 also exhibits superb long-term stability, water-resistance, and high thermal stability up to 650 °C.
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Bangxiang Liu,Hengjia Zhu,Jinjin Liu,Mengzhu Wang,Jianming Pan,Rulin Feng,Panwang Hu,Xiangheng Niu
As a typical antibiotic pollutant, tetracycline (TC) is producing increasing threats to the ecosystem and human health, and exploring convenient means for monitoring of TC is needed. Here, we proposed alkali-etched imprinted Mn-based Prussian blue analogues featuring superior oxidase-mimetic activity and precise recognition for the colorimetric sensing of TC. Simply etching Mn-based Prussian blue analogues (Mn-PBAs) with NaOH could expose the sites and surfaces to significantly improve their catalytic activity. Density functional theory calculations were employed to screen the molecularly imprinted polymer (MIP) layer for target identification. Consequently, the designed Mn-PBANaOH@MIP possessed the rich channels for substrates to get in touch with the active Mn-PBANaOH core, showing an excellent catalytic capacity to trigger the chromogenic oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) without the use of H2O2. If TC was introduced, it would be recognized selectively by the MIP shell and masked the channels for TMB access, resulting in the obstruction of the chromogenic reaction. According to this mechanism, selective optical detection of TC was achieved, and performance stability, reusability, and reliability as well as practicability were also verified, promising potential for TC monitoring in complex matrices. Our work not only presents an effective way to enhance the enzyme-like activity of Prussian blue analogues but also provides a facile approach for TC sensing. Additionally, the work will inspire the exploration of molecularly imprinted nanozymes for various applications.
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Materials Chemistry Frontiers
·
2023
·Vol. 7
·期 17
·3728-3737
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IF 7
Xiaohu Guo,Ke Yue,Jiale Zheng,Zaoli Yu,Yao Wang,Yujing Liu,Tiefeng Liu,Jianmin Luo,Xinyong Tao,Jianwei Nai
Improving overall water electrolysis efficiency is challenging due to difficulties in designing high-efficiency, non-noble metal oxygen evolution electrocatalysts. The key to success lies in improving the electrocatalyst's specific surface area and optimizing its electronic structure. In this study, a novel method for obtaining coronal manganese cobalt Prussian blue analogues (MnCo PBA) with high specific surface area was developed through simple chemical etching. The MnSe/CoSe2 composite, derived from coronal MnCo PBA, retains the high specific area characteristics of the precursor. The resulting coronal MnSe/CoSe2 demonstrates excellent OER performance, attributed to the high specific area composite MnSe/CoSe2, which exposes more active sites and promotes synergistic effects between its components. The overpotential at a current density of 10 mA cm−2 is 360 mV, and the electrocatalyst displays long-term stability of up to 200 hours. This work offers a unique and effective approach to designing high-performance OER electrocatalysts.
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CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Yue Zhao,Rui Gao,He Wang,Yanping Sun,Xiaohui Zhan,Lei Chen,Junyan Liu,Huixiang Shi
The adsorption and protective calcination methods were combined to synthesize single Mn atoms catalyst with more Mn-N x exposure for peroxymonosulfate (PMS) activation. During the carbonization process, the surface adsorbed Mn species in zeolitic imidazolate framework-8 (ZIF-8) and the surrounding graphitic carbon nitride (g-C 3 N 4 ) jointly maintained the morphology of precursor and enriched Mn-N 6 sites near the catalyst surface. The hollow and hierarchically porous structures induced by the erosive function of g-C 3 N 4 further facilitated the exposure of Mn-N 6 sites and mass transfer processes. Herein, the derived hollow carbon polyhedron catalyst (C-Z8-Mn@g-C 3 N 4 ) possessed highly accessible edge-host Mn-N 6 sites and ultra-high specific surface area (1846.91 m 2 g −1 ). C-Z8-Mn@g-C 3 N 4 exhibited remarkable catalysis for sulfamethoxazole (SMX) degradation at an extremely low dosage (0.01 g L −1 ), particularly, up to 3.8 times of promotion was obtained compared to traditional single Mn atoms catalyst (66.9 vs 17.8 L g −1 min −1 ). Besides, the catalytic performance of C-Z8-Mn@g-C 3 N 4 was not obviously affected by initial pH (3.14–11.00), inorganic anions and natural organic matters (NOMs). Experiments and Density functional theory (DFT) calculations revealed that Mn-N 6 sites not only had stronger PMS adsorption capacity than graphitic N, but also enhanced the electron transfer between catalyst and PMS, thus promoting the redox and self-decomposition of PMS to produce SO 4 − , OH and singlet oxygen ( 1 O 2 ) (as major active oxygen species). This work provides new insights into the regulation of active sites exposure in single-atom catalysts for enhanced catalytic performance.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Kangning Wang,Mengran Qin,Chuantao Wang,Ting Yan,Yanzhong Zhen,Xiaolei Sun,Jianwei Wang,Feng Fu
The construction of composite materials is an effective strategy to solve the problems of poor conductivity, manganese dissolution, and volume expansion of manganese-based materials. Herein, a CeO 2 /MnO x @C hollow composite cathode derived from the self-assembly of Ce-Mn-metal-organic frameworks (Ce-Mn-MOFs) was synthesized. The abundant oxygen vacancies and good electronic/ionic conductivity of CeO 2 improve the electrical conductivity of composite, enhancing the rate performance. The unique hollow structure could inhibit manganese dissolution and alleviate volume expansion. The results indicate that the 1 % CeO 2 /MnO x @C composite cathode possesses a high reversible capacity and excellent cycling stability. Specifically, the 1 % CeO 2 /MnO x @C composite cathode shows a remarkable reversible specific capacity of 130 mAh/g at a current density of 500 mA g −1 , 6.5 times more than the pure MnO x (20 mAh/g). The capacity retention is up to 99.5 % relative to the initial capacity after 800 cycles. This study provides a new strategy for designing rare-earth composite electrodes to improve electrochemical performance.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2022
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IF 10.753
Shuning Chen,Tengfei Ren,Xiaoying Zhang,Zuoyong Zhou,Xia Huang,Xiaoyuan Zhang
Heterogeneous catalytic ozonation (HCO) is attractive for water decontamination and catalyst is a core element. However, it is difficult to maintain high efficiency and stability of catalysts under stern conditions. In this study, we proposed Mn-loaded C-SiO 2 -Framework (Mn-CSF) which contained stable silica core and robust carbon shell for efficient catalytic ozonation. The pseudo-first-order kinetic rate constant for oxalic acid removal of Mn-CSF catalytic ozonation was 160 % and 875 % higher than those of Mn-SiO 2 and pristine CSF, respectively. Mn-CSF was also proven effective in gasification wastewater treatment , where the COD was decreased to 46 mg·L −1 , 37 % lower than that of Mn-SiO 2 . These results indicated that the graphitization carbon layer and Mn significantly enhanced the activity of the catalyst. Furthermore, a fulvic-like component and a protein-like component were recognized through 3D-EEM in coal gasification wastewater. It was proven that Mn-CSF catalytic ozonation exhibited higher fulvic-like component and protein-like component removal compared with ozonation. Moreover, O 2 − and 1 O 2 were identified to be responsible for organic degradation in this research. Sufficient external specific surface area and porous structure were important for complex wastewater treatment. Specifically, external specific surface area could enhance the degradation of macromolecular organics while porous structures were vital for smaller molecular pollutant removal . The results highlighted that Mn-CSF was a promising HCO catalyst for advanced wastewater treatment, and this study provided evidence of relationship between structure of catalysts and HCO efficiency.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Peipei Huang,Qing Chang,Guodong Jiang,Keru Xiao,Xu Wang
Metal organic frameworks are important Fenton-like materials in environment remediation. Nevertheless, the slow Fe(III)/Fe(II) cycling and low H 2 O 2 utilization limit their application. In this study, we develop the ferrous bimetallic MIL-101(Fe II 3 , Mn), which significantly enhanced catalytic performance (5.8 and 31.4-fold higher phenol removal rate and apparent rate constant, respectively) compared with the original MIL-101(Fe). The mechanisms are fully investigated by XPS, EPR and DFT. The Fe 2+ substitution affords the mixed-valences of Fe(III)/Fe(II) in the frameworks, which serve as stronger sites for H 2 O 2 activation. Mn in MIL-101(Fe II 3 , Mn) can also function as another reaction center to activate H 2 O 2 . Catalysts could coordinate with the π–electrons of pollutants, resulting in the electron transfer from pollutants to MIL-101(Fe II 3 , Mn). Moreover, electrons around Mn atoms tends to transfer to the region of Fe atoms owing to the electronegativity difference, inducing to strengthen the electron-rich Fe micro-region. Therefore, H 2 O 2 was primarily adsorbed onto electron-rich regions where it would be efficiently reduced to •OH, contributing to a higher H 2 O 2 utilization (81.2 %). This study opens new insight into design of Fe-based MOFs as highly efficient Fenton-like catalysts in wastewater treatment.
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Materials Today Energy
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2022
·
IF 9.257
Xianglei Liu,Changjian Yuan,Hangbin Zheng,Chao Song,Cheng Tian,Ke Gao,Nan Sun,Zhixing Jiang,Yimin Xuan,Yulong Ding
Calcium carbonate (CaCO 3 ) pellets are suitable for scalable solar thermochemical energy storage but suffer from low solar absorptance, poor stability, and slow reaction kinetics, which lead to low solar energy storage efficiency. Here, for the first time, we successfully achieve fast and efficient solar thermochemical energy storage via synergistically employing Al, Mn, and Fe stabilizers for improving both cyclic stability and solar absorptance, and Li 2 CO 3 promoters for accelerating decomposition of CaCO 3 pellets. The average solar absorptance is 1500% higher than that of pure CaCO 3 pellets. After 60 cycles, the energy storage density is still as high as 1671 kJ/kg with a decay rate of only 4.14%, in stark contrast to energy density of 1121 kJ/kg and decay rate of 56.73% for pure CaCO 3 pellets. The average decomposition rate is about twice as fast as that of pure CaCO 3 pellets due to enhanced Ca 2+ diffusion by doped Li 2 CO 3 . Under direct light irradiation, novel CaCO 3 pellets demonstrate high energy storage rate due to both high solar absorptance and fast decomposition rate, while pure CaCO 3 pellets cannot even reach the decomposition temperature. This work opens new opportunities for scalable deployment of direct solar-driven thermochemical energy storage techniques based on Li 2 CO 3 -doped dark CaCO 3 pellets.
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ACS Omega
·
2022
·
IF 4.132
Qingxiang Wang,Tao Huang,Jing Du,Lulu Zhou
The extraction of uranium (U)-related minerals from raw ore sands via a leaching procedure would produce enormous amounts of tailings, not only causing radioactivity contamination to surroundings but also wasting the potential U utilization. Effective recycling of U from U tailings is propitious to the current issues in U mining industries. In this study, the influence of the composite oxidation of Fe(III) and Mn(VII) intensified by microwave (MW) irradiation on the acid leaching of U from tailings was comprehensively explored in sequential and coupling systems. The U leaching activities from the tailing specimens were explicitly enhanced by MW irradiation. The composite oxidation caused by Fe(III) and Mn(VII) further facilitated the leaching of U ions from the tailing under MW irradiation in two systems. Maximum leaching efficiencies of 84.61, 80.56, and 92.95% for U ions were achieved in the Fe(III)-, Mn(VII)-, and Fe(III)–Mn(VII)-participated coupling systems, respectively. The inappropriateness of the shrinking core model (SCM) demonstrated by the linear fittings and analysis of variance (ANOVA) for the two systems explained a reverse increase of solid cores in the later stage of leaching experiments. The internal migration of oxidant ions into the particle cores enhanced by MW accelerated the dissolution of Al, Fe, and Mn constituents under acidic conditions, which further strengthened U extraction from tailing specimens.
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