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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Introducing different long-chain flexible ligands to regulate the transformation behavior of NiFe-MOF and as bifunctional catalysts for the HER/OER

Boyan Dai,Xinyu Wei,Liang Chen,Xiaolong Bao,Qin Zhong,Hongxia Qu

The investigation of highly efficient metal–organic framework (MOF) electrocatalysts represents a pivotal challenge in enhancing the overall efficiency of water electrolysis. In this study, we present a co-liganding method based on molecular regulation, in which succinic (s.a), adipic (a.a), and decanedioic (d.a) acids are employed to modify the original ligand H 2 BDC-based bimetallic NiFe-MOF to obtain dual-ligand NiFe-MOF electrocatalysts with excellent OER and HER performance (NiFe-MOF s.a, NiFe-MOF a.a, and NiFe-MOF d.a). Notably, NiFe-MOF d.a performs the best, particularly in 1 M KOH solution, with an OER overpotential of 242 mV and an HER overpotential of 116 mV at a current density of 10 mA cm −2 , and it demonstrates excellent stability under alkaline conditions, outperforming several recently reported Fe/Co/Ni-based catalysts. Bader charge and Mulliken charge calculations alongside experimental characterization data indicate that long-chain dicarboxylate ligands can influence the morphology, oxygen vacancy formation, and electronic structure of NiFe-MOFs. XPS and XRD analyses after the OER reveal that the four NiFe-MOFs undergo structural reorganization, with NiFe-MOF d.a having more unsaturated metal sites and more oxygen vacancies, promoting greater conversion of the MOF to NiOOH and FeOOH, which is beneficial for improving the OER performance. The density of states (DOS) results from DFT calculations demonstrate that the d-band center of NiFe-MOF d.a is relatively low, indicating that the adsorption energy of H* is reduced, which can promote the release of H 2 . Furthermore, the hydrogen adsorption free energy (ΔG H* ) values of the Fe and Ni active sites within NiFe-MOF d.a are closer to zero, thus accelerating the HER kinetics. This work paves new pathways for realizing dual-ligand MOFs.

研究领域: 材料科学 · 电化学
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SENSORS · 2020 ·Vol. 20 ·期 4 ·995 · IF 3.275

Preparation of “Ion-Imprinting” Difunctional Magnetic Fluorescent Nanohybrid and Its Application to Detect Cadmium Ions

Lina Chen,Yue Lu,Minshu Qin,Fa Liu,Liang Huang,Jing Wang,Hui Xu,Na Li,Guobao Huang,Zhihui Luo,Baodong Zheng

In this work, we have fabricated a novel difunctional magnetic fluorescent nanohybrid (DMFN) for the determination of cadmium ions (Cd2+) in water samples, where the “off-on” model and “ion-imprinting” technique were incorporated simultaneously. The DMFN were composed of CdTe/CdS core-shell quantum dots (QD) covalently linked onto the surface of polystyrene magnetic microspheres (PMM) and characterized using ultraviolet-visible spectroscopy (UV-Vis), fluorescence spectroscopy, and transmission electron microscopy (TEM). Based on the favorable magnetic and fluorescent properties of the DMFN, the chemical etching of ethylene diamine tetraacetic acid (EDTA) at the surface produced specific Cd2+recognition sites and quenched the red fluorescence of outer CdTe/CdS QD. Under optimal determination conditions, such as EDTA concentration, pH, and interfering ions, the working curve of determining Cd2+was obtained; the equation was obtained Y = 34,759X + 254,894 (R= 0.9863) with a line range 0.05–8 μM, and the detection limit was 0.01 μM. Results showed that synthesized magnetic fluorescent microspheres had high sensitivity, selectivity, and reusability in detection. Moreover, they have significant potential value in fields such as biomedicine, analytical chemistry, ion detection, and fluorescence labeling.Keywords:bifunctional;magnetic;fluorescent;Cd2+;detection;ion-imprinting

CAS / MDL: 25952-53-8
研究领域: 分析化学 · 材料科学 · 环境科学
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INORGANIC CHEMISTRY COMMUNICATIONS · 2022 · IF 3.428

Removal and recovery of phosphorus from solution by bifunctional biochar

Yunwen Liao,Si Chen,Qian Zheng,Bingyuan Huang,Juan Zhang,Hongquan Fu,Hejun Gao

The bifunctional biochar(N/CaO/BC) was prepared by a simple high temperature calcination using melamine and biomass material of sugarcane bagasse and agricultural wastes eggshell. Its structure and properties were analyzed by SEM, XRD, BET, and XPS. The adsorption capacity was evaluated in the phosphorus solutions. The effect of initial pH, concentration and temperature on adsorption were investigated. Nano-CaO were disperse evenly on the surface of Biochar, resulting a special specific surface area and porous structures. It has a rich nitrogen and CaO and the adsorption capacity could obtain 251.16 mg P/g at 300 K over a broad range of pH. The electrostatic force caused by C = NH + and precipitation reaction caused by CaO are the main driving forces of phosphorus removal and it exhibited a good P adsorption selectivity. P-rich N/CaO/BC contain P, N, C, Ca elements, which could provide nutrients to the soil and promotes the growth of crops. The dual-functionalization strategy of biochar provides a new way for the reuse of waste biomass and a new method for P utilization as resource in agricultural production.

研究领域: 环境科学 · 农业科学
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Sustainability · 2022 ·Vol. 14 ·期 20 ·13417 · IF 3.889

Ag Decorated Co3O4-Nitrogen Doped Porous Carbon as the Bifunctional Cathodic Catalysts for Rechargeable Zinc-Air Batteries

Pingshu Leng,Hanbin Wang,Binfeng Wu,Lei Zhao,Yijing Deng,Jinting Cui,Houzhao Wan,Lin Lv

The use of transition metals as bifunctional catalysts for rechargeable zinc-air batteries has recently attracted much attention. Due to their multiple chemical valence states, the cobalt oxides are considered to be promising catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). In this work, bifunctional Ag-decorated Co3O4-nitrogen doped porous carbon composite (Co3O4-NC&Ag) catalysts were synthesized by annealing ZIF-67 in N2and O2, respectively, followed by Ag deposition using chemical bath deposition. Due to the decoration of Ag nanoparticles and high specific surface area (46.9 m2g−1), the electrochemical activity of Co3O4increased significantly. The optimized Co3O4-NC&Ag catalysts possessed superior ORR performance with a half-wave potential of 0.84 V (vs. RHE) and OER activity with an overpotential of 349 mV at 10 mA cm−2. The open circuit voltage of the Co3O4-NC&Ag-based zinc-air battery was 1.423 V. Meanwhile, the power density reached 198 mW cm−2with a specific discharge capacity of 770 mAh g−1at 10 mA cm−2, which was higher than that of Pt/C-based zinc-air battery (160 mW cm−2and 705 mAh g−1). At a current density of 10 mA cm−2, the charge-discharge performance was stable for 120 h (360 cycles), exhibiting better long-term stability than the Pt/C&RuO2counterpart.Keywords:zinc air battery;Co3O4;bifunctional catalysts;silver decoration

研究领域: 材料科学 · 电化学
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BIOMASS & BIOENERGY · 2025 · IF 5.8

Enhanced conversion of CO2 to aromatics over spinel Mg3-XCrXO4 coupled HZSM-11 nanosheets bifunctional catalyst

Hui Hou,Jingang Yao,Fuli Yang,Hongqing Ma,Guiying Xu

CO 2 and green hydrogen for aromatics production are effective methods to mitigate CO 2 emissions. Herein, Mg 3-X Cr X O 4 spinel oxide was constructed via co-precipitation of Mg and Cr, followed by physical mixing with HZSM-11 to form a metal oxide-zeolite (OX-ZEO) bifunctional catalyst. The catalytic performance of this system in CO 2 aromatization was systematically evaluated. Notably, the designed catalysts followed a methanol-mediated pathway, overcoming limitations of the Anderson-Schulze-Flory distribution in aromatic hydrocarbon products. At varying Mg/Cr molar ratios, MgCr 2 O 4 /HZSM-11 exhibited the highest single-pass CO 2 conversion of 19.2 % and the highest aromatic selectivity of 75.2 % (excluding CO). Additionally, the optimal reaction conditions were determined for MgCr 2 O 4 /HZSM-11, achieving an excellent aromatic selectivity of 82.4 % and a CO 2 conversion of 22.6 % at 320 °C, a gas hourly space velocity (GHSV) of 1200 mL·gat −1 ·h −1 and a pressure of 3.5 MPa. After 100 h, the MgCr 2 O 4 /HZSM-11 tandem catalyst maintained substantial catalytic activity, with aromatic selectivity and CO 2 conversion of 79.3 % and 21.1 %, respectively. This strategy offers valuable insights for designing OX-ZEO bifunctional catalysts.

研究领域: 催化化学 · 环境科学 · 材料科学
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ACS Applied Nano Materials · 2024 · IF 5.3

Mn-Doped Crystalline Ni3S2/Amorphous MoS2 Core–Shell Nanorods as Bifunctional Electrocatalysts for Highly-Efficient Overall Water Splitting

Shaobo Ye,Zhentao Du,Zhengxiang Cai,Deliu Ou,Haonan Guo,Qiao Liu,Weiyou Yang,Qing Shi

Molybdenum disulfide (MoS2), a typical earth-abundant material, is an excellent candidate for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), which fundamentally rely on the regulation of the morphology and electronic structure of MoS2. Herein, Mn-doped amorphous MoS2 coated on Mn-doped crystalline Ni3S2 nanorods (Mn–Ni3S2@MoS2), rationally designed core–shell nanorods, have been fabricated via a facile one-step hydrothermal method as highly efficient bifunctional activities for HER and OER in alkaline solution. The target electrodes deliver a high current density of 100 mA cm–2 at a low overpotential of 187 and 310 mV for HER and OER, respectively, outperforming most MoS2-based catalysts. Moreover, a water-splitting cell based on the Mn–Ni3S2@MoS2 electrode requires a voltage of 1.45 V to reach a current density of 10 mA cm–2, which is superior to the state-of-the-art one of those based on noble metal Pt/C–NF∥RuO2–NF and non-noble metal catalysts. The overall enhanced bifunctional catalytic performance is mainly attributed to the abundant catalytically active sites provided by the Mn-doped amorphous MoS2 and the fast pathway for electron/proton transfer facilitated by the Mn-doped crystalline Ni3S2 nanorods. The incorporated Mn dopants and assembled Ni3S2/MoS2 heterostructure effectively regulate the electronic structure with redistributed charge within the core–shell Mn–Ni3S2@MoS2 electrode.

CAS / MDL: 12036-10-1
研究领域: 材料科学 · 电化学
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BIOTECHNOLOGY LETTERS · 2019 ·Vol. 41 ·期 10 ·1187-1200 · IF 2.154

Characterization of a bifunctional alginate lyase as a new member of the polysaccharide lyase family 17 from a marine strain BP-2

Huang Guiyuan,Wen Shunhua,Liao Siming,Wang Qiaozhen,Pan Shihan,Zhang Rongcan,Lei Fu,Liao Wei,Feng Jie,Huang Shushi

Objectives Bifunctional alginate lyase can efficiently saccharify alginate biomass and prepare functional oligosaccharides of alginate. Results A new BP-2 strain that produces alginate lyase was screened and identified from rotted Sargassum . A new alginate lyase, Alg17B, belonging to the polysaccharide lyase family 17, was isolated and purified from BP-2 fermentation broth by freeze-drying, dialysis, and ion exchange chromatography. The enzymatic properties of the purified lyase were investigated. The molecular weight of Alg17B was approximately 77 kDa, its optimum reaction temperature was 40–45 °C, and its optimum reaction pH was 7.5–8.0. The enzyme was relatively stable at pH 7.0–8.0, with a temperature range of 25–35 °C, and the specific activity of the purified enzyme reached 4036 U/mg. A low Na + concentration stimulated Alg17B enzyme activity, but Ca 2+ , Zn 2+ , and other metal ions inhibited it. Substrate specificity analysis, thin-layer chromatography, and mass spectrometry showed that Alg17B is an alginate lyase that catalyses the hydrolysis of sodium alginate, polymannuronic acid (polyM) and polyguluronic acid to produce monosaccharides and low molecular weight oligosaccharides. Alg17B is also bifunctional, exhibiting both endolytic and exolytic activities toward alginate, and has a wide substrate utilization range with a preference for polyM. Conclusions Alg17B can be used to saccharify the main carbohydrate, alginate, in the ethanolic production of brown algae fuel as well as in preparing and researching oligosaccharides.

研究领域: 海洋生物学 · 酶学 · 生物化学
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FUEL PROCESSING TECHNOLOGY · 2023 · IF 7.5

Enhanced conversion of syngas to high-quality gasoline hydrocarbons over ZnZrOx coupled SAPO-11 nanosheets bifunctional catalyst

Saisai Liu,Jing Liu,Guanyi Chen,Jingang Yao,Beibei Yan,Weiming Yi,Zhanjun Cheng,Chunyan Tian,Huijie Zao

Syngas is a key precursor for synthesizing gasoline (C 5 -C 11 ) hydrocarbons, offering an efficient route for utilizing non-petroleum carbon sources. However, the conventional Fischer-Tropsch synthesis (FTS) process faces a constraint with a maximum 45% selectivity for C 5 -C 11 , attributed to the Anderson-Schultz-Flory (ASF) distribution. Herein, bifunctional catalysts comprising ZnZrO x with different Zr/Zn ratios along with SAPO-11 zeolite sieves featuring varied morphologies like nanosheets (SA-A), petals (SA-B), and spheres (SA-C) have been effectively formulated and employed for the syngas-to-gasoline hydrocarbons (STG) reaction. Notably, the selectivity toward C 5 -C 11 far exceeded the ASF limits. Under identical reaction parameters, the Zn 1 Zr 4 O x /SA-A catalyst demonstrated notable enhancements of 6.6% and 26.2% in CO conversion, along with 4.6% and 7.6% increases in C 5 -C 11 selectivity, as compared to that of Zn 1 Zr 4 O x /SA-B and Zn 1 Zr 4 O x /SA-C catalysts, respectively. Furthermore, under the ideal conditions (380 °C, 4.5 MPa and gas hourly space velocity (GHSV) of 2400 mL min −1  g −1 ), Zn 1 Zr 4 O x /SA-A exhibited an exceptional C 5 -C 11 selectivity of 69.8% (CO 2 -free) alongside a single-pass CO conversion of 30.4%. Impressively, isoparaffin constituted 39.2% of the total composition , with the iso/n-paraffin ratio reaching 11.8. Even after 100 h, the catalyst maintained its remarkable catalytic activity , with the CO conversion and C 5 -C 11 selectivity maintaining levels of 27.5% and 66.85%, respectively.

研究领域: 化学工程 · 催化科学
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ACS Applied Materials & Interfaces · 2024 · IF 8.3

Morning Glory-Inspired Dual-Function Microcapsules for the Self-Reporting and Self-Healing of Electrothermal-Induced Damage of Electrical Devices

Potao Sun,Zhaoping Li,Wenxia Sima,Tao Yuan,Ming Yang,Kaisen Fan,Xiaoxiao Chen,Wenlong Pang

The long-term operation of power equipment and power electronics can cause local overheating and discharges in the insulation material, resulting in irreversible insulation damage. Further development of such damage can eventually lead to equipment failure, but this problem is very difficult to solve. In this paper, inspired by how the petals of morning glory change color with the environment due to the presence of pigmented globules, a dual-function heat alert in the form of a self-healing (HASH) microcapsule with a nested structure is prepared by using microfluidic technology. By combination of the microcapsule with the insulation material, the local overheating in equipment can be detected promptly under live operating conditions without manual external intervention, and the defects that occur can be repaired autonomously. These HASH microcapsules can be pre-embedded in places at which the material is prone to overheating using artificial magnetic targeting. The doping of the matrix material with microcapsules does not cause any deterioration in its electrical or mechanical properties. This technology is expected to be applied to electrical equipment and electronic devices to allow for the early detection of local overheating and the autonomous repair of defects, thereby ensuring the safety of the equipment and improving its service life.

研究领域: 材料科学 · 电气工程
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ACS Sustainable Chemistry & Engineering · 2024 · IF 7.1

Uncovering the Influence Mechanisms of H2O, O2, and NO2 on CeNiCa Dual-Function Material for Integrated CO2 Capture and In Situ Methanation

Linjia Li,Yiran Zhang,Jiaqi Feng,Shu Zhao,Wei Qiu,Ke Li,Zhen Huang,He Lin

Derived from carbon capture, utilization, and storage (CCUS), integrated carbon capture and utilization (ICCU) has been widely developed recently. Understanding the influences of H2O, O2, and NO2 on dual-function materials (DFMs) performance is crucial for their practical application. In this study, the influence mechanisms of O2, H2O, and NO2 on CeNiCa DFM for ICCU-methanation are investigated. The catalyst was oxidized by O2, H2O, and NO2. NO2 competes with CO2 for basic adsorption sites, inhibiting CO2 adsorption and methanation, but adsorbed NO2 is reduced mainly to N2 and NH3 during methanation. H2O induces agglomeration of the adsorbent and catalyst─the former due to the Ca(OH)2 mobility, and the latter attributed to OH-promoted migration and agglomeration of Ni. On this basis, it is proposed that the dominant roles of H2O, O2, and NO2 change in two- and multi-interference components, but the joint effects among them should not be neglected.

研究领域: 化学工程 · 环境科学
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Journal of CO2 Utilization · 2018 · IF 5.503

Highly selective conversion of CO2 to lower hydrocarbons (C2-C4) over bifunctional catalysts composed of In2O3-ZrO2 and zeolite

Jianyang Wang,Anfeng Zhang,Xiao Jiang,Chunshan Song,Xinwen Guo

Although many researchers have reported CO 2 hydrogenation to various C1 chemicals, it is still challenging to directly and selectively convert CO 2 to C 2 -C 4 hydrocarbons in terms of overcoming the extreme inertness of CO 2 and a high C C coupling barrier. In the present work, we report an efficient integration of methanol-synthesis and the methanol-to-hydrocarbons with the bifunctional catalyst component of In 2 O 3 -ZrO 2 and SAPO-5. These tandem reactions exhibit an excellent relative selectivity of C 2 -C 4 (83%) with a suppressed CH 4 relative selectivity less than 3% at T = 300 °C. A detailed analysis indicates that the partially reduced indium oxide surface (In 2 O 3 -ZrO 2 ) can better activate CO 2 and promote the synthesis of methanol than In 2 O 3 alone, and C C coupling is subsequently manipulated within the confined acidic pores of SAPO-5 according to XRD, H 2 -TPR, CO 2 -TPD, SEM and TEM. Furthermore, the proximity of two components and the content of Si also play an important role in such outstanding selectivity to C 2 -C 4 . Our study paves a new path for the direct synthesis of lower hydrocarbons.

CAS / MDL: 1314-23-4
研究领域: 化学工程 · 催化化学 · 能源化学
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Crafting amorphous VO2–crystalline NiS2 heterostructures as bifunctional electrocatalysts for efficient water splitting: The different cocatalytic function of VO2

Weiliang Zhou,Xiaojie Li,Xuan Li,Jiaxin Shao,Hengpan Yang,Xiaoyan Chai,Qi Hu,Chuanxin He

The rational design of bifunctional electrocatalysts is essential to achieve efficient hydrogen production from water splitting. Here, inspired by cocatalysts widely utilized in photocatalysis , we designed a heterostructure comprising amorphous VO 2 and crystalline NiS 2 , aiming at using VO 2 cocatalyst to boost activity of NiS 2 for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Intriguingly, we found that VO 2 displayed different co-catalytic function in boosting the OER and HER. Specifically, the VO 2 optimized the binding energy of hydrogen intermediate on NiS 2 and thus improved the HER activity. As for the OER, the amorphous VO 2 was easily dissolved in the KOH electrolyte, resulting in the generation of abundant oxygen vacancies in the in-situ generated active phase of NiOOH from NiS 2 , thereby drastically enhancing the OER activity. Consequently, the obtained VO 2 –NiS 2 @CC displayed excellent performance for overall water splitting, with a low voltage of 1.53 V at 10 mA cm −2 .

研究领域: 材料科学 · 催化化学
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