Molecular Catalysis
·
2024
·
IF 3.9
Zhan-Jun Zhu,Zhen-Hong He,Sen-Wang Wang,Bao-Ting Wu,Yue Tian,Yong-Chang Sun,Kuan Wang,Weitao Wang,Huan Wang,Zhao-Tie Liu
Compared with conventional thermal catalysis reaction, the photothermal CO 2 -assisted oxidative dehydrogenation of propane (CO 2 -ODHP) to produce propylene and CO is an environmentally friendly and sustainable method that operates at lower temperatures. In the present work, we have developed a series of Co-Mn/MCM-41 catalysts and utilized them in the photothermal CO 2 -ODHP reaction. Among these catalysts, the sample with Co and Mn loadings of 3 % resulted in activities of 225.7 μmol g cat −1 h −1 of propylene and 272.0 μmol g cat −1 h −1 of CO at 250 °C. Characterization results revealed that the electron transfer and interplay between Co and Mn oxides enhance the photoelectronic response and reduce impedance, facilitating the electron transfer process. Besides, the Co and Mn bimetallic species could enhance photothermal conversion efficiency and further enhance the local temperature during the reaction. The present work introduces a novel strategy for building supported bimetallic oxides in achieving CO 2 -ODHP via the photothermal route and is also expected to provide an optional catalyst required satisfactions including efficient electron transfer and photothermal conversion for other photothermal reactions.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2025
·
IF 5.4
Qing Chen,Ling Shi,Guiping Xu,Maocong Hu,Mao Peng,Zhenhua Yao
The development of low-cost and efficient bifunctional electrocatalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is of importance for the commercialization of green and sustainable energy conversion devices. In this work, noble metal-free XFeCoNiCu (X = Cr, Mg, and Mn) high entropy alloys were prepared with a facile pyrolytic reduction approach while the structure and composition were characterized by XRD, ICP-OES, TEM, HRTEM, and XPS. The prepared quinary alloys demonstrated excellent activity and stability for both ORR and OER, which was even superior to that of commercial Pt/C and RuO₂. Moreover, all three catalysts exhibited considerable potential for bifunctional catalysis, with a ΔE gap of 0.659 V for CrFeCoNiCu, a ΔE gap of 0.692 V for MnFeCoNiCu, and a ΔE gap of 0.727 V for MgFeCoNiCu, which was much better than that of the Pt/C+RuO 2 combination (0.723 V). The superior performance was further revealed by Density Functional Theory (DFT) calculations with projection density of states (PDOS) and free energy change. The strategy proposed in this study provides an economical approach to design and develop bifunctional electrocatalysts with exceptional performance.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Jia-Ying Zhang,Lin-Feng Zhai,Sheng-Nan Tang,Hao-Li,Zhuo-Feng Hu,Min Sun
This study presents a novel nonradical catalytic oxidation system for targeted p-hydroxybenzene sulfonate (PHS) production from sulfonamides (SAs). A positive external electric field was applied to induce the in-situ activation of O 2 on Mn-doped Co 3 O 4 surface, with Mn-doping used to manipulate the reactivity of surface complexes. Theoretical simulations predicted CoMn-peroxides as thermodynamically favorable candidates for the targeted PHS production. Experimental validation achieved PHS yields of 18.4–32.6 % from five typical SA compounds. While 1 O 2 also actively participated in the oxidation of SAs, disruption of the 1 O 2 oxidation pathway significantly enhanced the PHS yields to 47.6–50.3 %. The intensity of electric field regulated the O 2 activation pathways by influencing the stability of CoMn-peroxides. This nonradical catalytic oxidation system demonstrated excellent catalyst reusability and environmental robustness for energy-efficient SAs removal and PHS recovery. These findings provide new insights into leveraging nonradical = pathways to advance catalytic oxidation technology for sustainable water management.
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Journal of Energy Storage
·
2024
·
IF 8.9
Huajing Zhang,Chao Xu,Xiangyu Sun,Bowen Xu,Zhirong Liao,Huawei Liu
Ca-based materials are considered to be promising energy storage materials for the 3rd generation concentrated solar power (CSP) plants due to their high energy storage density , high operating temperature , and low energy loss . However, the poor cyclic stability, low solar absorption capability, and slow reaction kinetics of conventional Ca-based materials seriously limit large-scale applications. Here, we successfully synthesized a Zr-Mn co-doped CaO-based composite, achieving good cyclic stability, enhanced solar absorption capability, and fast carbonation reaction kinetics simultaneously. The energy storage performance of 20Ca-0.5Zr-0.5Mn was evaluated at a high carbonation reaction temperature of 850 °C. Results showed that the performance decay of 20Ca-0.5Zr-0.5Mn was only 10.11 % over 30 cycles. By co-doping Zr and Mn elements, the carbonation reaction kinetics of CaO-based composites were promoted because of increased basicity and oxygen vacancies . Compared with pure CaO, the average solar absorptance of 20Ca-0.5Zr-0.5Mn was enhanced by about 376 %. Therefore, the proposed Zr-Mn co-doped CaO-based composite indicates the bright applied prospect in CSP plants for solar energy storage .
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Kaiting Chen,Qingwei Li,Xinyu Han,Cheng Rao,Xiangguang Yang,Yibo Zhang
Developing efficient low-temperature selective catalytic reduction (CO-SCR) catalysts remains a key challenge in reducing nitrogen oxide (NOx) emissions. Here, we report a photothermal-enhanced Rh–Mn/CoAlOx heterostructure catalyst that achieves excellent NO conversion (more than 90% at 140 °C) and N2 selectivity (>80%) under visible to infrared light irradiation. By integration of highly dispersed Rh units with Mn clusters onto a hydrotalcite-derived CoAlOx support, the catalyst exhibits synergistic light absorption and dynamic lattice oxygen migration capabilities. Through combined analysis using in situ DRIFTS, XAFS, XPS, EPR, and other techniques, we reveal that Mn doping induces numerous oxygen vacancies and promotes electron transfer between Rh and Mn, facilitating lattice oxygen activation via a mechanism similar to the Mars-van Krevelen mechanism. Light exposure reduces the activation energy and, according to Arrhenius analysis and NO-TPD results, accelerates the decomposition of nitrate intermediates and enhances the conversion rate of nitrous oxide to N2. Density functional theory (DFT) calculations confirm that N2O is more likely to be generated at the Rh–Mn interface, demonstrating its enhanced low-temperature activation ability for NO. This study innovatively enhances the catalytic performance of CO-SCR using light, providing a sustainable method for reducing low-energy NOx emissions.
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ACS Applied Energy Materials
·
2025
·
IF 5.5
Zhu-Yu Li,Le-Ran Li,Tong Wu,Qi Niu,Bing Zhang,Ji Liu,Kai Li,Qiang Lu
Calcium-looping-based thermochemical energy storage (TCES) technology can be embraced for peak load shifting in renewable energy generation systems. However, the energy storage properties of Ca-based materials rapidly decay after multiple cycles. In this study, a synergistic strategy involving pyroligneous acid impregnation and Mn–Co–Al incorporation was developed to improve the pore structure, enhance the oxygen vacancy concentration, and boost antisintering performance of the calcium-based composites, thereby significantly improving their TCES properties and cyclic durability. The modified CaO-based composites were systematically analyzed using various characterization methods to evaluate their heat storage performance, sintering resistance mechanism, and physicochemical properties. Characterization results revealed that the codoped sample with Ca:Mn:Co:Al = 100:12:4:5 (PACa-Mn12Co4Al5) possessed a loose and porous surface with a measured specific surface area of 13.72 m2/g, providing channels for CO2 diffusion into the inner particles. Ca3CoMnO6 and Ca3Al2O6, acting as inert supports, were uniformly distributed in PACa-Mn12Co4Al5, effectively mitigating sintering. The addition of Mn–Co–Al strengthened the basicity and promoted oxygen vacancy formation in PACa-Mn12Co4Al5. The oxygen vacancies encouraged the formation of ion diffusion channels, reducing the O2– transport resistance across the surface and within the bulk of PACa-Mn12Co4Al5, thereby improving the reaction activity and conversion efficiency. PACa-Mn12Co4Al5 demonstrated excellent heat storage performance under calcination at 750 °C and carbonation at 850 °C. After 40 and 100 cycles, its energy storage density remained at 97.29% and 84.65% of the initial value (1212.79 kJ/kg), respectively. Moreover, the average radiation absorptance of PACa-Mn12Co4Al5 reached 59.85%, 5.26 times that of limestone-based CaO. Therefore, PACa-Mn12Co4Al5 is a promising heat storage material, providing guidance for the industrial application of Ca-based TCES materials.
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ENVIRONMENTAL RESEARCH
·
2025
·
IF 7.7
Bo Song,Zhenxing Shen,Qingzhu Tian,Guiling Zhou,Qin Peng,Hao Fan,Jia Liu
Volcanic rock is a natural mineral with a porous structure and rich in various metal oxides. It has been used in environmental applications such as water and soil pollution remediation as stable chemical properties and low cost. In this work, volcanic rock was used in the field of nitrogen oxide control, and the feasibility of preparing NH 3 - Selective Catalytic Reduction catalyst was evaluated. The catalyst AVR-10Mn-450 was prepared by acidification-impregnation-calcination process, and it can achieve more than 90 % denitration effect at 175 °C, 25000 h −1 . It removes nitrogen oxides through the Eley–Rideal and Langmuir–Hinshelwood pathways. AVR-10Mn-450 has the advantages of simple preparation and low cost compared with the mainstream nano-denitration catalysts. It can be applied to the pretreatment of industrial flue gas such as cement plant or glass plant, thereby extending the service life of the precious metal or nano-catalyst at the back end. This work not only realizes the high-value resource utilization of volcanic rock, but also reduces the production cost of denitration catalyst.
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WATER AIR AND SOIL POLLUTION
·
2025
·Vol. 236
·期 10
·1-14
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IF 3
Liu Jingliang,An Fengxia,Zheng Di,Li Chao,Sun Jingya
In this study, Mn-Ni-layered double hydroxides (Mn-Ni-LDHs) were synthesized and utilized to activate peroxymonosulfate (PMS) for degrading reactive brilliant blue KN-R (KN-R) in aqueous solutions. The characterization results demonstrate that the catalysts synthesized are layered structures, and the surface area is 169.3 m 2 /g. The Mn-Ni-LDHs exhibited significant efficiency effective for the degradation of KN-R via activating PMS, achieving 96.5% degradation of KN-R within 90 min under optimal conditions (0.20 g/L catalyst, 10 mM PMS, pH=10.0 and 25°C). The reaction followed pseudo-first-order kinetics with a rate constant of 0.0351 min -1 , and the apparent activation energy was calculated to be 11.94 kJ/mol. Electron paramagnetic resonance (EPR) and free radical scavenging experiments identified ·O 2 − and 1 O 2 as the primary reactive species involved in the reaction for KN-R degradation. The proposed catalytic mechanism suggests that redox cycling between Mn 4+ /Mn 3+ and Ni 3+ /Ni 2+ within Mn-Ni-LDHs plays a critical role in enhancing PMS activation, thereby promoting the continuous generation of active oxygen species.
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Surfaces and Interfaces
·
2025
·
IF 6.3
Qingtao Zeng,Bingjie Zhang,Shengzhi Jiao,Mingyue Gao,Ruyu Li,Haiyan Xiao,Longgang Wang
The emergence of nanozymes based on metal-organic frameworks has successfully addressed some limitations of natural enzymes. ZIF-8 is a framework with high pore rate consisting of Zn 2+ and 2-methylimidazole, but its catalytic activity is limited. In this study, a new metal organic framework named ZIF-8 (FM) was prepared by doping iron and manganese in ZIF-8, which exhibited enhanced catalytic performance. ZIF-8(FM) showed the peroxidase-like (POD-like) activity by oxidizing chromogenic substrates and was capable of colorimetric detection of dopamine in actual samples. In addition, in order to improve the photothermal conversion efficiency, ZIF-8(FM) was wrapped with polydopamine (PDA) to prepare ZIF-8(FM)@PDA. The antibacterial experiments of Escherichia coli and Staphylococcus aureus showed that ZIF-8(FM)@PDA had strong antibacterial effect. Nanomaterials based on ZIF-8(FM) have great potential in dopamine detection and effective photothermal antibacterial treatment.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Xue Luo,Yingying Xue,Leilei Xu,Linshui Lian,Cai-e Wu,Yan Cui,Weixin Zou,Lin Dong,Fei Gao,Mindong Chen
This study presents a systematic investigation into the catalytic oxidation of toluene using metal–organic framework (MOF)-derived porous metal oxide catalysts obtained through controlled pyrolysis. The MOF-derived catalysts (Mn3O4-BTC, CeO2-BTC, Co3O4-BTC) demonstrated remarkable improvements in catalytic activity and stability compared to their commercial counterparts (Mn3O4-c, CeO2-c, Co3O4-c), achieving 90% toluene conversion (T90) at significantly lower temperatures of 240 °C, 241 °C, and 237 °C, respectively. Besides, a comprehensive suite of characterization techniques was employed to elucidate the structure–activity relationships. Specifically, various traditional and in situ characterization techniques, including X-ray diffraction (XRD), N2 physisorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), H2 programmed reduction (H2-TPR), online-tandem thermogravimetry-mass spectrometry (online-tandem TG-MS), and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS), were employed to elucidate crystallinity, porosity, morphology analysis, probe surface chemistry, redox properties, real-time tracking of thermal decomposition, and reaction mechanisms during the catalytic oxidation of toluene. It was found that the enhanced catalytic performance could be attributed to the synergistic effects of a high surface area, well-dispersed active sites, and abundant oxygen vacancies. These insights provided fundamental insights into the design and optimization of MOF-derived catalysts for efficient volatile organic compounds (VOCs) abatement in environmental catalysis.
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NMR IN BIOMEDICINE
·
2025
·Vol. 38
·期 9
·e70116
·
IF 2.7
Fei-Xiang Hu,Deng-Deng Liu,Xiao-Wen Ma,Pu-Yeh Wu,Wei-Jun Peng,Dan Wang,Tong Tong
This study aims to design and evaluate a two-dimensional Ti 3 C 2 -MXene contrast agent, codoped with iron and manganese, with the aim of achieving T 1 /T 2 dual-mode magnetic resonance imaging contrast, and to investigate its effect on Chemical Exchange Saturation Transfer (CEST) contrast agents. Single-layer Ti 3 C 2 was synthesized via the HCL/LiF etching technique, with the flake size subsequently tailored and the hydroxylated surface modified through a hydrothermal process. Fe 3 O 4 nanoparticles and MnO 2 nanosheets were integrated onto the two-dimensional Ti 3 C 2 -MXene surface using an in situ doping approach, and the final modification was achieved with carboxymethyl chitosan. Various characterization techniques were employed to assess the physical and chemical properties of the probe, which were then combined with a CEST contrast agent to investigate the mechanisms of multimodal magnetic resonance imaging and in vitro photothermal effects. Upon integrating the multi-modal molecular probe with Ioversol for imaging purposes, at a magnetic field strength of B 1 = 1.25 μT and with a molecular probe concentration of 0.5 mg/mL, the CEST signal from Ioversol is almost entirely suppressed. This allows for the successful identification of a distinct concentration range where both contrast agents can coexist. In vitro photothermal studies on MXene codoped with iron and manganese have shown that the composite molecular probe exhibits excellent photothermal efficiency. The method combining complex nanoprobes with CEST contrast agents successfully achieved simultaneous imaging of both contrast agents. In vitro MRI experiments successfully obtained distinguishable concentration ranges for both, with changes in CEST signals reflecting the concentration variations of the complex molecular probes, which also exhibit good photothermal therapy (PTT) capabilities.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Li-Ming Sun,Bin Li,Ang Li,Ze-Zhou Ding,Xin-Hui Wang,Yu-Xi Huang,Chang Liu,Tong Li,Wei-Sheng Huang,Xing Zhang
The Mn–Co dual-metal oxide is recognized as an effective activator for peroxymonosulfate (PMS), but its activation mechanism remains controversial. In this study, a Co/Mn–C–N (CMCN) nanocatalyst was synthesized using a simple pyrolysis method, and its catalytic activity along with the PMS activation mechanism was comprehensively explored. The findings indicated that the synergistic effect of Mn and Co within the bimetallic composition significantly enhanced the catalytic efficiency of CMCN compared to those of individual metal oxides (Mn–C–N and Co–C–N). Bisphenol A underwent successful degradation within 3 min in a neutral environment, with a degradation kinetic rate of 1.59 min–1 and a total organic carbon removal efficiency of 63.8%. Moreover, CMCN nanoparticles demonstrated remarkable stability and reusability, maintaining their efficacy over four cycles. Employing a series of experiments and analytical characterizations, a novel activation mechanism for PMS was proposed, involving both radical and nonradical pathways. This mechanism involves the oxidation of organic pollutants through a direct electron transfer process from metastable intermediate complexes. Notably, the CMCN/PMS system exhibited a robust resistance to interference factors. This research provides novel insights into the development of bimetallic oxide composites for the effective removal of recalcitrant water pollutants.
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