CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Jiamei Xiang,Yan Lu,Huizi Li,Rujuan Tang,Renjie Zhang
Constructing stable and highly active asymmetric Mn N 3 single-atomic sites integrated with Mn nanoclusters remains challenging. This work develops a facile secondary pyrolysis strategy to fabricate a porous dual-site catalyst (Mn SA /Mn NC -NC) featuring both single-atom Mn N 3 (Mn SA ) and Mn nanoclusters (Mn NC ) sites on nitrogen doped carbon black (NC). The Mn NC not only stabilizes the Mn SA but also enhances the overall conductivity and preserves the hierarchical porous framework, thereby maximizes dual-site exposure and mass transport. This synergy endows Mn SA /Mn NC -NC with outstanding activity for bifunctional oxygen catalysis with half-wave potential of 0.91 V and onset potential of 1.59 V, both surpassing those of commercial noble metal Pt/C and RuO 2 . A liquid zinc-air battery (LZAB) assembled with Mn SA /Mn NC -NC achieves a high power density of 218.0 mW cm −2 and stability exceeding 500 h. Density functional theory (DFT) calculations insightfully reveal the inherent mechanism that Mn NC not only stabilizes asymmetric Mn SA , but also precisely modulates the electronic structure and d-band energy levels, which kinetically optimizes the desorption behavior of reaction intermediates *OH and thermodynamically lowers the reaction energy barrier. This work verifies the critical role of nanoclusters on asymmetric single-atom sites, offering essential guidance to design of high performance catalysts for energy storage devices.
✓ 已验证
DOI
高影响因子
AICHE JOURNAL
·
2023
·Vol. 69
·期 9
·e18149
·
IF 3.7
Yongxiao Tuo,Ying Meng,Qing Lu,Qing Wang,Furong Jia,Yan Zhou,Xiang Feng,Jun Zhang,Xuezhi Duan,De Chen
The enhancement of catalytic activity is always limited by the dilemma in activation and desorption due to Sabatier principle. Locating the Sabatier optimum by manipulating catalyst electronic structure has been a long-standing challenge in heterogeneous catalysis. Herein, we presented a generic strategy to continuously tailor the Pt 5d state occupancy via tuning the Pt O Mn electronic linkage over Al 2 O 3 -confined MnO x islands, aiming at accommodating the C H cleavage and product desorption capabilities in dehydrogenation of liquid organic hydrogen carriers (monocyclic/bicyclic hydrides). Rising Mn valence can decrease the Pt 5d state occupancy through more electron transfer from Pt 5d to O 2p due to the strong π-donation of O 2p to Mn 3d. This will lead to the lower initial C H activation energy barrier while higher product desorption energy barrier. An intermediate Pt 5d filling of ~8.4 in Pt Mn 2 O 3 /Al 2 O 3 enables the balanced level of product desorption and C H activation, thus ensuring a superior dehydrogenation activity. The electron structure-adsorption-performance modulation mechanism described herein provides a benchmark to locate the Sabatier optimum for the metal catalyst design.
✓ 已验证
DOI
高影响因子
Symmetry-Basel
·
2023
·Vol. 15
·期 7
·1334
·
IF 2.7
Guolin Song,Chengzhu Shen,David Bassir,Qiulin Li
In this study, a facile strategy of regulated self-assembly synthesis of Mn-MIL-100, using sodium acetate (CH3COONa) as a mono-dentate ligand capping agent (CA), was proposed. The as-prepared product is denoted Mn-MIL-100-CA. The coordination modulation of CH3COONa, led by its interference in the connectivity and symmetry of the metal centers and organic nodes, plays a vital role in the synthesis process. The crystallinity, morphology, topology, and properties of such MOF products were improved, since the self-assembly process of Mn-MIL-100-CA was promoted and regulated effectively. The materials were systematically characterized via XRD, SEM, N2isotherms, XPS, and TGA in terms of crystallization behavior, morphology, topology, chemical composition, and thermal and water stability. The ability of Mn-MIL-100 and Mn-MIL-100-CA to remove methylene blue (MB) from an aqueous solution was investigated using a UV–vis spectrophotometer. The results indicate that with the addition of a molar ratio of 50% CH3COONa, Mn-MIL-100-CA particles developed a regularly symmetrical morphology, i.e., ‘spherical pyramid-like structure’ crystals with a dimension of 2~5 μm. Their specific surface area and pore volume increased by 59.2% and 56.7%, respectively. The increased proportion of Mn3+implies reduced crystal defects and improved crystal structural order and integrity, and therefore an enhanced water stability. Mn-MIL-100-CA exhibited excellent adsorption performance towards MB from aqueous solution. The equilibrium adsorption value was as high as 1079.9 mg/g, which is 44.7% higher than that of Mn-MIL-100 without the addition of CA. The good adsorption capacity and excellent water stability mean that Mn-MIL-100-CA has great potential for the practical removal of MB dye pollutants from water.Keywords:metal organic frameworks;Mn-MIL-100;capping agent;symmetry;self-assembly;methylene blue adsorption
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Honghong Lyu,Pin Li,Jingchun Tang,Weixin Zou,Pengfei Wang,Bin Gao,Lin Dong
Synergy between adsorption and photocatalysis provides an ideal green technology to treat antibiotic pollution in water. In this study, single-atom Mn anchored on N-doped graphene oxide (Mn-NGO) was synthesized for enhanced adsorptive-photocatalytic removal of aqueous sulfanilamide (SNM) and the corresponding mechanisms were revealed. The Mn-NGO had better performance of SNM degradation and TOC removal than GO and NGO. Density functional theory (DFT) calculation showed that the electrons of d-orbital (Mn) and p-orbital (N) upgraded the electronic structures of GO of the Mn-NGO to interact with amino and aromatic rings of SNM, increasing the adsorption and polarizing of SNM. Furthermore, more hydroxyl and superoxide radicals were observed on Mn-NGO, leading to the generation of key reaction intermediates of 2-aminohydroquinone and benzenesulfonic and thus subsequently opening loops and mineralizing SNM. In addition, Mn-NGO effectively removed SNM in different types of water systems (e.g., lake water, tap water, and deionized water) through synergistic adsorption-photocatalytic degradation.
✓ 已验证
产品关联
DOI
高影响因子
ACS Biomaterials Science & Engineering
·
2022
·
IF 5.395
Wei Ma,Huanli Zhang,Shuying Li,Zhiqiang Wang,Xiaodan Wu,Rui Yan,Fang Geng,Weijie Mu,Yingxue Jin
Chemodynamic therapy (CDT) based intracellular chemical reactions to produce highly cytotoxic reactive oxygen species has received wide attention. However, low efficiency of single CDT in weakly acidic pH and glutathione (GSH) overexpressed tumor cells has limited its clinical application. For this study were prepared two-dimensional metal–organic framework (MOF) to improve CDT efficiency based on the combined action of bimetallic CDT, consumption of overexpressed glutathione (GSH) in cells, folic acid (FA) induced tumor targeting and triphenylphosphine (TPP) induced mitochondrial targeting. With the use of Cu(II) as the central ion and tetrakis(4-carboxyphenyl)porphyrin (TCPP) as the ligand, two-dimensional Cu-MOF nanosheets were prepared, which were surface modified by manganese dioxide based on the in situ redox reaction between poly(allylamine hydrochloride) (PAH) and KMnO4 to obtain Cu-MOF@MnO2. Then FA and TPP were coupled with the nanosheets to form the title nanoplatform. Comprehensive physiochemical research has suggested that Cu(II) and MnO2 constituents in the nanoplatform could consume intracellular GSH and hydrogen peroxide to generate hydroxyl radicals through a Fenton-like reaction; meanwhile Cu(II) could undergo a Russell reaction to produce cytotoxic singlet oxygen. Detailed in vitro and in vivo biological experiments have revealed a good biosafety profile and a high tumor suppression effect. Therefore, the present research has realized multiple and efficient CDT effects with the aid of the sequential targeting of FA/TPP, also providing a strategy for the development of CDT drugs based on polymetallic organic frameworks.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Tuo Wang,Yifei Cao,Huimin Wu,Chuanqi Feng,Yu Ding,He Mei
In this work, N-Ni 1 Co 3 Mn 0.4 O/NF is synthesized as multifunctional electrocatalyst for hydrogen evolution (HER), urea oxidation reaction (UOR) and hydrazine oxidation reaction (HzOR). The optimal Ni/Co (molar ratio) and the amount of doping Mn are investigated, the sample with Ni/Co = 1:3 and the addition of 0.4 mmol Mn exhibits the best catalytic activity with the largest specific surface area. Then the two-electrode electrolyzers composed of N-Ni 1 Co 3 Mn 0.4 O/NF are constructed, and the results from experiments show that the voltage required for overall hydrazine splitting (OHzS) at 100 mA cm −2 is 0.272 V, 1.614 V lower than that of overall water splitting (OWS, 1.886 V), while the overall urea splitting (OUS) needs 1.669 V, 0.187 V lower than that of OWS, revealing the outstanding thermodynamic and kinetic advantages of OUS and OHzS. The superior performance may be attributed to the heterostructure between metal and metal oxide and N-doping, which can promote electron transfer and optimizes the decomposition of urea and hydrazine hydrate and hydrogen production , and the research on mechanism will be carried out in the future.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF LUMINESCENCE
·
2021
·
IF 3.599
Kewei Ma,Yuhang Sheng,Guizhen Wang,Xiaowei Zhang,Yunsong Di,Cihui Liu,Liyan Yu,Lifeng Dong,Zhixing Gan
Mn 2+ doping has been developed to modulate the photoluminescence (PL) of CsPbCl 3 perovskite quantum dots (PQDs). However, the doped Mn 2+ may be expelled from the PQDs host with the long-term storing, resulting in inferior stability. Herein, CsPbCl 3 PQDs doped with different concentrations of Mn 2+ (Mn:CsPbCl 3 ) are prepared by a hot injection method. Our photostability tests reveal that when the doping concentration is <25%, or 40%–50%, the Mn 2+ doped PQDs are intrinsically stable. Anion exchange reactions are conducted between the stable CsPb 0.796 Mn 0.204 Cl 3 and CsPbBr 3 PQDs. Fluorescence color gamut of the resulting Mn:CsPb(Cl/Br) 3 PQDs almost covers the entire visible spectrum except for the deep red color. Benefiting from the intrinsic stability and wide color gamut, multicolor solid-state luminescence are acquired by incorporating the Mn:CsPb(Cl/Br) 3 PQDs in polymethyl methacrylate (PMMA) matrices, which are used as color converters for constructing light-emitting diodes (LEDs) with different colors.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yeyin Zhang,Ruting Huang,Yong Fang,Jiacheng Wang,Zijie Yuan,Xinwei Chen,Wenjie Zhu,Yuan Cai,Xianyang Shi
This study developed metal–organic frameworks (MOFs) with enhanced properties for CO 2 conversion by doping second- transition metal ions (Ti, Mn, Zn, and Cu) into Fe–MOF, which resulted in Fe-M−MOF (M = Ti, Mn, Zn, or Cu). The selection of different metal species in the metal cluster nodes of the MOFs significantly impacted the CO 2 conversion efficiency. Among the different combinations, the Fe–Cu bimetallic cluster node was identified as the most optimal node. In addition, we investigated various variables and preparation conditions for determining the optimal synthesis conditions for Fe–Cu-MOFs. We observed that a synthesis temperature, time, and pH of 130 °C, 15 h, and 3.2, respectively, yielded the best results. The 13 CO 2 isotope labeling method confirmed that the carbon source of CO and CH 4 were derived from CO 2 . Under simulated visible-light irradiation (λ ≥ 420 nm), Fe–Cu-T130 exhibited the highest photocatalytic activity, with a CH 4 generation rate of up to 444.2 μmol g −1 h −1 . This high activity was attributed to several factors. First, the presence of Fe 2+ , Fe 3+ , and Cu 2+ on the surface of Fe–Cu-T130 resulted in photogenerated electrons and holes under visible-light excitation. Fe 2+ accepted electrons to reduce CO 2 , whereas Fe 3+ and Cu 2+ oxidized H 2 O through holes. Second, the polycrystalline structure of Fe–Cu-T130 with abundant surface oxygen vacancies enhanced the chemical reactivity. Finally, the low conduction band position and narrower bandgap of Fe–Cu-T130 facilitated the excitation of electrons into the conduction band, thereby promoting the CO 2 reduction reaction. This study successfully demonstrated the enhanced photocatalytic activity of Fe–Cu-T130 for CO 2 conversion under visible light. The findings provide insight into the development of MOFs with improved properties for the sustainable and efficient utilization of CO 2 .
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Yao Deng,Yanmei Li,Jing Wang,Huidi Zhang,Lin Wang,Qiong Wang,Tao Xu,Wenlei Wang
Nitrogen deficient porous nanosheets(NDCN) are a promising nano template that can combine defect engineering with Mn-FeOOH to suppress photo generated carrier complexation and optimize electron distribution . In this study, a unique structure with N/O double vacancies in Mn-FeOOH@NDCN was prepared using a magnesium thermal denitrification co-precipitation method. Furthermore, a series of Mn-FeOOH/NDCN/PMS reaction systems were constructed by adjusting the dosage of peroxymonosulfate(PMS). The experimental results indicate that the synergistic activation of N/O double vacancies on PMS enables the Mn-FeOOH/NDCN/PMS system to oxidize almost 10 mg/L of As(III) within 90 min. At the same time, the oxidized As(V) was completely adsorbed, thereby completely removing the total arsenic in the water. The reasonable construction of carbon networks is a prerequisite for the stability of Mn-FeOOH/NDCN composite catalysts, enabling them to have good cyclic stability. The experimental results confirm that oxygen vacancies directly participate in the activation of PMS, while nitrogen vacancies effectively adsorb As(III), thereby promoting the contact between As(III) and PMS, improving the mass transfer rate, and accelerating the catalytic degradation process. This study will provide a new way to completely remove arsenic pollution from water bodies.
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Prosper Kwame Klu,Muhammad Abdul Nasir Khan,Chaohai Wang,Junwen Qi,Xiuyun Sun,Jiansheng Li
Development of efficient catalysts for peroxymonosulfate (PMS) activation and further understanding its mechanism on organic pollutants degradation is of significant importance for advanced oxidation processes (AOPs). Herein, hollow (Co, Mn) 3 O 4 catalysts were synthesized by calcination of Co, Mn containing metal-organic frameworks (MOFs) and further used to evaluate the effectiveness of organic pollutants (Bisphenol A (BPA), atrazine (ATZ), and diethyl phthalate (DEP)) degradation by PMS activation. The PMS utilization efficiency in (Co, Mn) 3 O 4 /PMS system (36.4%) was estimated to be 28.0% and 43.8% higher than that of Co 3 O 4 /PMS and Mn 5 O 8 /PMS system, respectively. Notably, the metal leaching in (Co, Mn) 3 O 4 /PMS system was significantly suppressed. The utilization efficiency also reveals an inverse proportionality relationship with BPA mineralization but decreases with increasing initial pH value. A synergy between oxides of Co and Mn was perceived to enhance PMS utilization efficiency and BPA degradation. The results indicate enhanced catalytic performance with (Co, Mn) 3 O 4 compared to Co 3 O 4 derived from Co-MOF and other reported catalysts, with 99% of BPA degradation within 4 min. The oxidation mechanism was then proposed based on the electron paramagnetic resonance (EPR) and XPS results. Our findings might have contributed to designing heterogeneous catalysts for efficient PMS utilization in AOPs.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF DRUG TARGETING
·
2021
·
IF 5.121
Yongwei Hao,Cuixia Zheng,Qingxia Song,Hongli Chen,Wenbin Nan,Lei Wang,Zhenzhong Zhang,Yun Zhang
Drug delivery with the help of nanoparticles could transport more payloads to tumour site. Owing to their limited accumulation and penetration in the tumour tissues, to increase delivery efficiency is currently still required for applying nanomedicine to treat tumour. Here, we initially report a pressure-driven accumulation of drug-loaded nanoparticles to tumours for efficient tumour therapy with a dry cupping device. The mesoporous Mn-doped silica based nanoparticles delivering 5-aza-2-deoxycytidine and docetaxel were prepared, characterised and used as a model nanomedicine to investigate the potential of dry cupping treatment. For this system, the Mn doping not only endowed the mesoporous silica nanoparticles biodegradability, but also made it much easier to bind a tumour targeting group, which is a G-quadruplex-forming aptamer AS1411. On tumour-bearing mice, the in vivo results demonstrated that the dry cupping treatment could substantially improve the distribution of nanomedicines at tumour site, resulting in enhanced treatment efficacy. Overall, this method enables the therapeutical nanoparticles accumulate to tumour through increasing the blood perfusion as well as altering the biological barrier, which opened up possibilities for the development of pressure-driven nanomedicine accumulation at tumour site.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2021
·Vol. 31
·期 13
·2007877
·
IF 18.808
Feng Chen,Xi-Lin Wu,Chenyang Shi,Hongjun Lin,Jianrong Chen,Yanpeng Shi,Shaobin Wang,Xiaoguang Duan
Heterogeneous Fenton-like reactions (HFLR) are promising alternative strategies to address the inherent limitations of the classic Fenton systems. Herein, a facile and scale-up approach for the synthesis of transition metal single-atom sites (SA-TM, TM = Cr, Mn, Fe, Co, Cu) coordinated onto pyrrolic N-rich g-C 3 N 4 (PN-g-C 3 N 4 ) scaffold is developed. The regulated pyrrolic N-rich SA-TM catalytic sites exhibit excellent performances for HFLR. As a model of SA-TM/PN-g-C 3 N 4 , SA-Cr/PN-g-C 3 N 4 is efficient for the catalytic oxidation of bisphenol A via HFLR under visible light with outstanding cyclic stability and wide effective pH range (3.0–11.0). The synergy of photocatalysis and single-atom catalysis leads to accelerated production and separation of charge carriers as well as the cycling of Cr 3+ /Cr 2+ couple, consequently boosting the performance in HFLR. Theoretical calculations indicate that the Cr(II)-N 4 sites with the metalloporphyrin-like structure are more reactive than the doped Cr(II) sites in the g-C 3 N 4 matrix, which act as the peroxidase-mimicking nanozyme for efficient and homolytic cleavage of peroxide O O in H 2 O 2 . This study expands the family of the iron-free Fenton-like systems and provides new strategies to the rational design and precise regulation of on-demand multifunctional single-atom catalysts for advanced water remediation.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）