Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Long Daojun,Liu Yongduo,Ping Xinyu,Chen Fadong,Tao Xiongxin,Xie Zhenyang,Wang Minjian,Wang Meng,Li Li,Guo Lin,Chen Siguo,Wei Zidong
The serious problem of carbon monoxide (CO) poisoning on the surface of Pt-based catalysts has long constrained the commercialization of proton exchange membrane fuel cells (PEMFCs). Regeneration of Pt sites by maintaining CO scavenging ability through precise construction of the surface and interface structure of the catalyst is the key to obtaining high-performance CO-resistant catalysts. Here, we used molybdenum carbide (MoC x ) as the support for Pt and introduced Ru single atoms (SA-Ru) at the Pt-MoC x interface to jointly decrease the CO adsorption strength on Pt. More importantly, the MoC x and SA-Ru are immune to CO poisoning, which continuously assists in the oxidation of adsorbed CO by generating oxygen species from water dissociation. These two effects combine to confer this anode catalyst (SA-Ru@Pt/MoC x ) remarkable CO tolerance and the ability to operate stably in fuel cell with high CO concentration (power output 85.5 mW cm −2 @20,000 ppm CO + H 2 – O 2 ), making it possible to directly use the cheap reformed hydrogen as the fuel for PEMFCs.
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Catalysis Science & Technology
·
2024
·Vol. 14
·期 3
·667-672
·
IF 4.4
Qiulan Huang,Ruiqin Ren,Jia Li,Muhammad Waqas,Pan Chen,Xiaotian Liu,Dujuan Huang,Zhongyun Yang,Xinglan Peng,Du-Hong Chen,Youjun Fan,Wei Chen
Fabricating highly competent and cost-effective catalysts is essential for promoting the sluggish kinetics associated with the oxygen reduction reaction (ORR). Herein, a new type of Fe, Co decorated porous carbon composite catalyst co-doped with S and N (FeCo–SNC) was prepared by a simple carbonization process. Interestingly, FeCo–SNC inherits not only the pore structure but also the large surface area of the ZIF-67 dodecahedron. Furthermore, the electronic configuration of the two catalytic centers in Fe–N–C and Co–NC was customized. On the basis of synergetic coordination between the two active sites, the fabricated FeCo–SNC showed prior stability for the ORR even after 10 000 cycles of cyclic voltammetry measurement, besides the great limiting current density of 5.99 mA cm−2 and high half potential of 0.856 V (vs. reversible hydrogen electrode), surpassing the commercially available Pt/C catalyst. Moreover, the primary active site of Fe–N–C was regulated, providing the highest catalytic activity for the ORR. This research offers a new perspective on enhancing carbon-based catalysts for the ORR without relying on precious metals and introduces a strategic method for controlling active centers.
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MOLECULES
·
2024
·Vol. 29
·期 10
·2349
·
IF 4.2
Ziwei Deng,Wei Liu,Junyuan Zhang,Shuli Bai,Changyu Liu,Mengchen Zhang,Chao Peng,Xiaolong Xu,Jianbo Jia
A Fe-Co dual-metal co-doped N containing the carbon composite (FeCo-HNC) was prepared by adjusting the ratio of iron to cobalt as well as the pyrolysis temperature with the assistance of functionalized silica template. Fe1Co-HNC, which was formed with 1D carbon nanotubes and 2D carbon nanosheets including a rich mesoporous structure, exhibited outstanding oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalytic activities. The ORR half-wave potential is 0.86 V (vs. reversible hydrogen electrode, RHE), and the OER overpotential is 0.76 V at 10 mA cm−2with the Fe1Co-HNC catalyst. It also displayed superior performance in zinc–air batteries. This method provides a promising strategy for the fabrication of efficient transition metal-based carbon catalysts.
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EUROPEAN JOURNAL OF PHARMACEUTICS AND BIOPHARMACEUTICS
·
2024
·
IF 4.4
Xianzhi Liu,Luyan Shen,Lin Zhou,Wencheng Wu,Guang Liang,Yunjie Zhao,Wenqi Wu
Developing co-amorphous systems is an attractive strategy to improve the dissolution rate of poorly water-soluble drugs. Various co-formers have been investigated. However, previous studies revealed that it is a challenge to develop satisfied acidic co-formers, e.g., acidic amino acids showed much poorer co-former properties than neutral and basic amino acids. Only a few acidic co-formers have been reported, such as aspartic acid , glutamic acid , and some other organic acids . Thus, this study aims to explore the possibility of adenosine monophosphate and adenosine diphosphate used as acidic co-formers. Mebendazole, celecoxib and tadalafil were used as the model drugs. The drug-co-former co-amorphous systems were prepared via ball milling and confirmed using XRPD. The dissolution study suggested that the solubility and dissolution rate of the drug-co-formers systems were increased significantly compared to the corresponding crystalline and amorphous drugs. The stability study revealed that using the two nucleotides as co-formers enhanced the physical stability of pure amorphous drugs. Molecular interactions were observed in MEB-co-former and TAD-co-former systems and positively affected the pharmaceutical performance of the investigated co-amorphous systems. In conclusion, the two nucleotides could be promising potential acidic co-formers for co-amorphous systems.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yi Fang,Shoubing Chai,Zhiwei Chu,Zirui He,Yingjie Li
In the calcium looping CO 2 capture process, using CO in the flue gas to reduce NO at a high molar ratio of CO to NO (e.g., above 10:1) can achieve efficient removal of NO. However, the lots of unreacted CO causes secondary pollution. In this study, a novel Cu/Ce co-modified CaO was proposed for cyclic CO 2 capture and the catalytic NO reduction at a low CO:NO molar ratio (e.g., 2:1). The experimental findings indicate that Cu/Ce modification improves the performance of CaO in both catalytic NO reduction and carbonation. The Cu/Ce co-modified CaO contained the optimal Cu/Ce/Ca molar ratio of 1:5:100 possesses both NO removal and CO conversion efficiencies of above 99 %, along with CO 2 removal efficiency exceeding 88%. Microscopic analysis determines that the electron transfer between Cu and Ce facilitates the conversion of lattice oxygen into surface oxygen, mitigating the competition between CO 2 and CO for surface oxygen. Furthermore, density functional theory calculations demonstrate that CO/NO/CO 2 exhibits non-competitive adsorption behavior on Cu/Ce co-modified CaO. Consequently, Cu/Ce-modified CaO possesses superior catalysis for efficient NO reduction by CO at low CO:NO molar ratio in calcium looping process.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Zhenfei Wang,Congli Li,Lei Tang,Jiahui Yang,Qi Shi,Jinxiang Dong
Ni-MOF-74 is among the most promising candidates for CO adsorption due to its highest CO adsorption capacity. However, the feasibility of using Ni-MOF-74 in actual CO/N2 pressure swing adsorption (PSA) processing cannot be reliably inferred based solely on its adsorption capacity at normal temperature and pressure. Hence, we systematically studied its CO working capacity and regenerability at different test temperatures and pressure ranges by single-component static and binary-component dynamic (CO/N2, 50%/50% and 30%/70%, v/v) experiments. The static experiments preliminarily indicated an appropriate operating temperature of 100 °C with adsorption–desorption pressures in the range of 3.0–0.1 bar for the PSA process. The working capacity and regenerability of CO were evaluated as 3.41 mmol·g–1 and 66.21% (adsorption–desorption pressure: 3.0–0.1 bar, 100 °C). A higher temperature reduces the binding force between CO and Ni-MOF-74, so that more CO is desorbed, which leads to an increase in the working capacity and regenerability of CO. Furthermore, through CO/N2 binary-component dynamic breakthrough experiments, the optimal operating temperature and CO adsorption partial pressure for the PSA process were determined as 100 °C and 1.5 bar at a total desorption pressure of 0.2 bar. Typically, for a CO/N2 composition of 50%/50%, the CO working capacity and regenerability were 2.66 mmol·g–1 and 85.25% at 100 °C and a CO partial pressure of 1.5 bar (total CO adsorption pressure of 3.0 bar) at a total desorption pressure of 0.2 bar. These results may guide PSA process design and optimization for adsorbents with strong CO binding ability.
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JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Jiaxin Huang,Huanbin Gou,Jinming Pan,Yuping Liu,Ming Nie,Bo Shang,Danmei Yu,Guangsheng Huang,Dingfei Zhang,Fusheng Pan
Within the domain of metal-air battery systems, developing the non - precious metal catalysts featuring extraordinary catalytic activity in oxygen reduction reaction (ORR) is crucial to the air-cathode. This work unveils a sol-gel engineered synthesis of La 0.9 Ce 0.1 Co 0.1 Mn 0.9 O 3 perovskite via the co-doping strategy, with targeted exploration of its electrochemical behavior and underlying mechanism in Zn-air and Mg-air battery systems. The perovskite La 0.9 Ce 0.1 Co 0.1 Mn 0.9 O 3 has a wealth of catalytically active ORR sites and a mesoporous architecture. The diffusion-limited current density of La 0.9 Ce 0.1 Co 0.1 Mn 0.9 O 3 successfully achieves a 1.2-fold enhancement relative to commercial Pt/C with a low H 2 O 2 yield of <0.27 %, underscoring its superior mass transport kinetics. The maximum power densities of La 0.9 Ce 0.1 Co 0.1 Mn 0.9 O 3 -based primary/secondary zinc - air batteries are 130 and 83 mW cm −2 , respectively, which are on a par with those of Pt/C - based Zinc - air batteries. Whereas, the open - circuit voltage and maximum power density of the primary magnesium - air battery fabricated with 10 wt% KCl as the electrolyte are 1.85 V and 52 mW cm −2 , respectively, which exhibit superiority over Pt/C catalysts. In combination with DFT analyses, the La 0.9 Ce 0.1 Co 0.1 Mn 0.9 O 3 perovskite emerges as a prospective ORR catalyst for metal-air battery realization.
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Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Shuya Rui,Na Liu,Lingwei Ren,Yang Liu,Zian Liu,Binghui Wu,Hua Pan,Zhiping Ye
Traditional Mn-Ce catalysts for selective catalytic reduction (SCR) of NO with CO (CO-SCR) in iron and steel flue gases are often hindered by competitive adsorption of NO and CO, which compromises catalytic efficiency. In this study, we present a Ni-doped Mn-Ce catalyst that overcomes these challenges, achieving 96 % NO conversion, 98 % N 2 selectivity, and 44 % CO conversion at 175 °C. Comprehensive characterization of the catalyst reveals that Ni doping significantly enhances Mn-Ce interactions, boosting oxygen vacancy density and promoting efficient redox cycling between Mn 3 + /Mn 4+ and Ce 3+ /Ce 4+ . Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) confirms preferential NO adsorption at oxygen vacancy sites, minimizing CO-NO competition and stabilizing the Langmuir-Hinshelwood mechanism, where both gases co-adsorb and react at oxygen-rich vacancies. Mechanistic insights suggest that Ni facilitates electron transfer, weakening the N–O bond in NO and accelerating its dissociation, resulting in faster NO reduction. This study establishes Ni doping as a promising strategy for improving the low-temperature performance of Mn-Ce-based CO-SCR catalysts, paving the way for more efficient catalytic systems.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Le Zhang,Xin Zhou,Shaohua Chai,Jian Guan,Guijun Fan,Wuxinchen Yang,Guojun Ma,Ning Han,Yunfa Chen
There is a high demand to synthesize ozone decomposition catalysts especially in high-space-velocity and high-relative-humidity (RH) environments. Herein, two polymorphs of cobalt hydroxide, α- and β-Co(OH)2, are synthesized and applied for ozone elimination. β-Co(OH)2 shows ∼90% ozone decomposition efficiency under high space velocity (weight hourly space velocity (WHSV) = 1,200,000 mL g–1 h–1, 25 °C, 40 ppm), which is far higher than that of α-Co(OH)2 (∼5%). β-Co(OH)2 has high spin Co(II) in distorted octahedral coordination caused by the Jahn-Teller effect, leading to a higher crystal field splitting energy level and thus contributing to the easier electron transfer between the ozone and catalyst. Moreover, β-Co(OH)2 still shows high performance (∼87%) even in humid conditions (RH ∼50%, 25 °C, 40 ppm, WHSV = 600,000 mL g–1 h–1), which is attributable to its abundant surface non-hydrogen-bonded hydroxyls weakening water molecule adsorption, providing an idea to develop highly efficient catalysts for ozone decomposition in humid environments.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Tan Hu,Yang Xu,Gang Xu
Self-assembling dipeptide hydrogels are attracting attention in food, materials, and biomedicine. However, there are still limitations such as weak hydrogel properties. Herein, we introduced two types of polysaccharides (Arabic gum and citrus pectin) into an alkyl-chain modified dipeptide (C 13 -tryptophan-tyrosine (C 13 -WY)) to generate co-assembled C 13 -WY-arabic gum and C 13 -WY-pectin hydrogels. The co-assembled hydrogels exhibited enhanced mechanical properties and stability. The G' value of C 13 -WY-arabic gum and C 13 -WY-pectin hydrogels was 3 and 10 times larger than that of C 13 -WY hydrogel, respectively. The addition of Arabic gum and citrus pectin led to the co-assembly and molecular rearrangement. Moreover, co-assembled hydrogels showed more β-sheet structure and hydrogen bonds. Importantly, the self-/co-assembled hydrogels showed low cytotoxicity. We utilized these hydrogels for the encapsulation of docetaxel and they showed a high embedding rate and slow-release. Our findings provide a novel strategy for the development of stable supramolecular peptide hydrogels with good biocompatibility through simple co-assembly.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2022
·Vol. 139
·期 29
·e52647
·
IF 3.057
Jinrong Yin,Yunlei Gong,Huaan Zheng,Hui Yuan,Zhen Zeng,Wei Qin,Chenghao Li,Yang Zhou,Xianyan Ren
Ultra-low-density proppants are of great significant in slick water fracturing system, but the polymer composite microspheres can hardly promise the quality of oil and gas due to their poor hydrophobicity. To address the issue, we prepared several types of modified styrene-divinyl benzene copolymer microspheres (MSDBs) with long-term durable hydrophobicity and high strength, including O-MSDBs (hydrophobic MSDBs), LO-MSDBs (long-time hydrophobic MSDBs), and CO-MSDBs (coated O-MSDBs) on the basis of a molecular structure of “KH570-styrene (St)-divinyl benzene (DVB)” copolymer. In this article, the design concept and the structure of MSDBs was clarified, and performances of MSDBs are systematically discussed and compared with commercially available hydrophobic microspheres. The O-MSDBs, a kind of nanoparticle patterned St-DVB copolymer microspheres, were prepared by a one-step suspension polymerization undergoing a sol–gel process, showing strong hydrophobicity with a water contact angle up to 140.7°, but short durability in strong hydrochloric acid or hydrofluoric acid; On the contrary, LO-MSDBs perform better in the stability and durability of hydrophobicity with a slightly lower water contact angle about 135.9°. The LO-MSDBs were designed by coating functionalized St-DVB copolymer microspheres with fluororesin. Similarly, CO-MSDBs from fluororesin-coated O-MSDBs were designed. As expected, CO-MSDBs have a stronger hydrophobicity (139.0°) than LO-MSDBs and longer durability than O-MSDBs. Moreover, the MSDBs exhibit better properties than the commercially available hydrophobic polymer and ceramic microspheres.
研究领域:
材料科学
·
石油工程
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Nano Energy
·
2021
·
IF 17.881
Dongdong Li,Qian Zhang,Zhichuan Shen,Kumar Siddharth,Lijuan Chen,Minhua Shao,Zhicong Shi
Rechargeable lithium oxygen batteries (LOBs) are one of the most promising energy storage systems by virtue of their high energy density and environmental amiability. However, the development of LOBs is still hindered by some critical issues. Herein, 3D hexapod-shaped Co-ZIFs-thiourea/dimethyl sulfoxide (H-Co-ZIFs-S) derived Co nanoparticles embedded into nitrogen and sulfur co-doped carbon (H-Co-NSC) are developed, and then low content of ruthenium nanoparticles are decorated on the surface to obtain Ru/H-Co-NSC as efficient catalyst for LOBs. The Ru/H-Co-NSC catalysts exhibits unique structure and catalytic properties , such as accommodating the insoluble discharge product Li 2 O 2 , promoting the transportation of ions/O 2, enhancing the electronic conduction, demonstrating excellent OER/ORR kinetics as well. In addition, the Ru-decorated nanoparticles could effectively suppress some side-reactions caused by the exposed carbon of H-Co-NSC in LOBs. First-principles Density functional theory (DFT) calculations reveal the cooperative effect of multiple active sites in Ru/H-Co-NSC can effectively promote the ORR/OER kinetics in LOBs. Therefore, the LOBs with Ru/H-Co-NSC cathode provide a positive catalytic capacity with low overpotential, large specific capacities, long cycle life and superior reversibility . Our work may pave the way to design more advanced catalysts for metal-air batteries with superior electrochemical performance.
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