International Journal of Electrochemical Science
·
2023
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IF 1.5
Changshui Wang,Jiahui Zhang,Caiyan Shi,Dandan Cai
The development of an inexpensive, efficient and robust water oxidation catalyst is important to achieve water splitting for renewable energy production. Herein, nickel-cobalt layered double hydroxides (Ni-Co LDHs) were rationally synthesized by a facile method and can be served as efficient electrocatalysts for water oxidation. For comparison, Ni-Co LDH nanoflowers have also been synthesized by controlling the synthetic process. The composition and morphologies of the catalysts were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FESEM) and X-ray photoelectron spectroscopy (XPS). The as-obtained Ni-Co LDH nanocages exhibit a high catalytic activity toward the water oxidation reaction (WOR). The electrochemical results show that the overpotential of Ni-Co LDH nanocages electrode was 350 mV at a catalytic current density of 10.0 mA cm -2 in 1.0 M KOH. Moreover, the Tafel slope was as low as ~ 93 mV dec -1 . The unusual catalytic properties of Ni-Co LDH nanocages could be attributed to the hollow structure and the synergetic effect between Ni metal and Co metal.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Yiqi Cui,Shuaikang Ying,Hongzhong Cai,Yan Wei,Changyi Hu
Carbon-supported platinum (Pt) for oxygen reduction reaction plays an important role in the operation of direct methanol fuel cells (DMFCs). However, complete oxidation of ethanol is difficult due to the low chemical activity of Pt / C. Herein, novel highly active Pt-Co/C nanoparticles with controllable chemical composition and particle size are prepared via a thermal reduction method. The results revealed that the catalyst (particle size: 2–4 nm) is characterized by a good size monodispersity, and exhibits satisfactory chemical activity. The nanoparticles were also characterized by an accurate and maintained stoichiometry ratio, resulting in improved electrocatalytic activity and anti-poisoning ability of the carbon-supported Pt.
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Yanni Shen,Xueli Miao,Dandan Song,Yanting Li,Yuning Qu,Jianguo Yu,Jiajun Tang,Hao Qin,Lili Wang,Jiahao Ren,Bing Wang
A facile and novel one-step hydrothermalmethod was provided for the preparation of Ni-Co double hydroxides (NC-DH), which was directly grown on carbonized cotton cloth (CCC) and used as advanced binder-free electrodes for supercapacitors. The effect of different concentration of Ni 2+ and Co 2+ in the intial reactant (C-Ni-x-Co-y) on microstructure and electrochemical performance were studied. The results showed that flake-like structure grown uniformly under an appropriate concentration, which was benefit to improve the electrochemical performance. The electrochemical tests revealed that the C-Ni-4-Co-8 electrode displayed the maximum specific capacitance of 4.19 F cm -2 when the current density was 5 mA cm-2and excellent rate capability maintained at 3.05 F cm -2 even at the high current density of 80 mA cm -2 . The electrodes of Ni-Co double hydroxides anchored on flexible conductive substrates with excellent electrochemical properties could be obtained by cost-effective method, which could be ascribed as a highly promising potential electrode material for energy storage devices.
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Yuying Zhao,Qixin Yuan,Kang Sun,Ao Wang,Ruting Xu,Jing Xu,Yan Wang,Mengmeng Fan,Jianchun Jiang
Carbon material is considered a promising electrocatalyst for the CO2 reduction reaction (CO2RR); especially, N-doped carbon material shows high CO Faradic efficiency (FECO) when using pyridinic N species as the active site. However, in the past decade, more efforts were focused on the preparation of various carbon nanostructures containing abundant pyridinic N species and few researchers studied the electronic structure modulation of the pyridinic N site. The curvature of the carbon substrate is an easily controllable parameter for modulating the local electronic environment of catalytic sites. In this research, carbon nanotubes (CNTs) with different diameters are applied to modulate the electronic environment of pyridinic N by the curvature effect. The pyridinic N sites doped on CNTs with the average curvature of 0.04 show almost 100% FECO at the current density of 3 mA cm–2 at −0.6 V vs RHE and 91% FECO retention after 12 h test, which is superior to most of the carbon-based electrocatalysts. As demonstrated by density functional theory simulation, the pyridinic N site forms a strong local electric field around the nearby C active site and protrudes out of the curved CNT surface like a tip, which remarkably enriches the protons around the adsorbed CO2 molecule.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Tongyi Shang,Xinying Yu,Yuan Gu,Rong Du,Yanjun Cai,Yuwei Li,Guodong Zheng,Chaoqun Wang,Jian Zhang,Jifang Liu,Shisong Han,Bin Yang
Cancer immunotherapy is the most promising method for tumor therapy in recent years, among which the macrophages play a critical role in the antitumor immune response. However, tumor-associated macrophages (TAMs) usually display the tumor-promoting M2 phenotype rather than the tumor-killing M1 phenotype. Moreover, the over-expressed CD47 on tumor cells severely hinders the function of macrophages by blocking the CD47/SIRPα pathway. Herein, a nano-assembly system of CHTR/siRNA was constructed through the host-guest interaction of a hyperbranched amino-functionalized β-cyclodextrin and immune agonist imiquimod (R848), while CD47 siRNA was loaded inside through electrostatic interaction. The Toll-like receptor (TLR) 7/8 agonist R848 can “re-educate” macrophages from the protumoral M2 phenotype to antitumoral M1 phenotype, while CD47 siRNA can down-regulate the “don't eat me” CD47 signal on the surface of cancer cells and enhance the phagocytosis of cancer cells by macrophages. Through the dual regulation of TAMs, the immunosuppressive tumor microenvironment was relieved, and the host-guest drug-carrying system resulted in synergistic immunotherapy effect on tumors and inhibited tumor growth. The facile self-assembly of nanodrug offers a new strategy in co-delivery of multiple therapeutic agents for cascade cancer immunotherapy.
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BIOCHEMICAL ENGINEERING JOURNAL
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2023
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IF 3.9
Chang Li,Zixuan Li,Yan Sun
Laccase , a green biocatalyst , has been widely used in the field of biodegradation with the assistance of electron mediators. Herein, a novel strategy, polyethyleneimine (PEI)-induced biomimetic mineralization , was explored and applied to co-immobilize laccase and 2,2′-azino bis (3-ethylbenzothiazoline)-6-sulfonic acid (ABTS). With the PEI doping, calcium phosphate (CaP) could facilely mineralize within 20 min to form PEI@CaP; ABTS could be co-mineralized with PEI to form (PEI + ABTS)@CaP. Laccase, a negatively charged protein, was then immobilized via electrostatic adsorption onto the embedded PEI in the carriers. Both of the immobilized laccase preparations, denoted as Lac-PEI@CaP and Lac-(PEI + ABTS)@CaP, showed high activity recoveries (96.4 % and 88.0 %, respectively), and increased pH tolerance and storage stability as compared to free laccase. ABTS and laccase loading densities of Lac-(PEI + ABTS)@CaP reached 0.83 mmol g −1 and 100 mg g −1 , respectively. Lac-(PEI + ABTS)@CaP presented higher malachite green (MG) degradation capability than free laccase and Lac-PEI@CaP with free ABTS, possibly due to the proximity effect of the co-immobilized laccase and ABTS. Moreover, Lac-(PEI + ABTS)@CaP exhibited reusability and kept 83.2 % of MG degradation activity after three recycles and 37.9 % in the sixth. This work provided a new strategy for the co-immobilization of laccase and electron mediator, and demonstrated the potential of the biocatalyst for organic pollutant removal.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Fangfang Fan,Qiulan Huang,Karuppasamy Kohila Rani,Xinglan Peng,Xiaotian Liu,Limin Wang,Zhongyun Yang,Dujuan Huang,Rajkumar Devasenathipathy,Du-Hong Chen,Youjun Fan,Wei Chen
The fabrication of highly efficient bifunctional catalyst for oxygen evolution/reduction reaction (OER/ORR) is essential for high performance rechargeable Zn-air batteries. Herein, we present a method of simultaneous interface/doping engineering to prepare bifunctional oxygen electrocatalyst for rechargeable Zn-air batteries. The Fe-Co 2 P/Co heterostructure was covered by N-doped carbon boxes (Fe-Co 2 P/Co@NC), and the surface electronic structure of Fe-Co 2 P/Co@NC was tailored through the controlled co-doping of P and Fe. Theoretical calculation revealed a significant charge accumulation at the interface of Fe-Co 2 P and Co, demonstrating a strong synergy in Fe-Co 2 P/Co@NC catalyst. The as-prepared Fe-Co 2 P/Co@NC catalyst exhibited an excellent catalytic performance for ORR/OER as well as rechargeable Zn-air batteries with large power density (783 mA h g Zn −1 ), high open circuit voltage (1.54 V) and long charge/discharge stability (155 h). This work provides a new approach for the construction of interface-rich heterostructure electrocatalysts for oxygen catalysis.
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FUEL
·
2023
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IF 7.4
Jinchuan Wang,Li Zhang,Jinping Weng,Juntao Wei,Deliang Xu,Bin Li,Shu Zhang,Mortaza Gholizadeh,Electo Silva Lora,Hong Zhang
The retention and transformation of nitrogen in hydrochars prepared from co-hydrothermal carbonization (Co-HTC) of fiberboard (FB) and glucose were mainly investigated in this study. This study showed that more than 90 wt% nitrogen has transferred into aqueous solution at 180–220 °C during the hydrothermal carbonization (HTC) of FB. When the HTC temperatures were higher than 220 °C, some dissolved nitrogen recombined into hydrochars due to the enhancement of nitrogen fixation reactions (Maillard reactions). The addition of glucose could significantly increase nitrogen retention rate in hydrochars, which was due to abundant oxygen-containing intermediates (5-HMF, furfural, etc.) formed in aqueous phase by the hydrothermal decomposition of glucose. Besides, the hydrochars with more microspheres formed on the surface could apparently enhance nitrogen fixation due to the increased contacting area. In Co-HTC, the temperature range of 220–280 °C favored the nitrogen retention in hydrochars. Additionally, nitrogen retention rate increased significantly with increasing residence time and mixture ratio of glucose in a certain extent. While the heterocyclic-N was the main nitrogen functional group in hydrochars and it transformed from pyridinic-N, pyrrolic-N to quaternary-N with higher HTC temperatures and longer residence times, additionally, some amine-N was clearly formed when the nitrogen returned from the aqueous phase into hydrochars.
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ELECTROCHIMICA ACTA
·
2023
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IF 6.6
Sun Lina,Sun Liping,Huo Lihua,Zhao Hui
The production of hydrogen peroxide (H 2 O 2 ) through electrochemically reducing O 2 in a two-electron pathway is a potential substitute for the traditional process based on anthraquinone. In this paper, F doping is carried out to prepare N and F co-doped porous carbon embedded Co nanoparticles. The electro-catalytic activity for the electrochemical production of H 2 O 2 is systematically investigated. The composite material demonstrates exceptional electro-catalytic selectivity, reaching approximately 92.5%, and shows an ultra-high rate of producing H 2 O 2 in 4021.4 mmol g -1 h -1 at 0.1 V versus RHE in a 0.5 M H 2 SO 4 electrolyte. It is found that the synergetic effect of Co-Nx and F in the composite material result in its exceptional performance. Adding F atom modulates the Zeta potential of the catalyst and alters the electronic configuration around Co-Nx, creating favorable conditions for the uptake of O 2 and consequently forming OOH*. Additionally, the highly electronegative F atom facilitate desorbing OOH* through electrostatic repulsion, preventing any further degradation. In a homemade electrolyzer containing 80 mg L -1 of Rh B, the H 2 O 2 produced in situ in a 0.5 M H 2 SO 4 electrolyte degrades up to 97.76% of Rh B in just 22.5 min, showcasing its potential for practical wastewater treatment applications.
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Catalysts
·
2023
·Vol. 13
·期 7
·1031
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IF 3.9
Jie Lin,Yihong Ding,Huile Jin,Tianbiao Zeng
Nickel, cobalt, and manganese oxides are easily obtainable non-noble metal catalysts for water splitting. However, the relationship between composition and catalysts’ performance still needs systematic studies. Herein, guided by theoretical calculations, a low overpotential, easily prepared Mn-doped Co3O4was deposited on graphite plates for water splitting. The 30% Mn-doped Co3O4(Co2.1Mn0.9O4) required the lowest overpotential for oxygen evolution reaction (OER), in which the Co2.1Mn0.9O4reached 20, 30, and 50 mA cm−2in the overpotentials of 425, 451, and 487 mV, respectively, with 90% IR compensation. Under overall water-splitting conditions, the current density reached 30 mA cm−2at an overpotential of 0.78 V without IR compensation. Charge density difference analysis illustrates that doped Mn provides electrons for O atoms, and that Mn doping also promotes the electron fluctuation of Co atoms. XPS analysis reveals that Mn-doping increases the chemical valence of the Co atom, and that the doped Mn atom also exhibits higher chemical valence than the Mn of Mn3O4, which is advantageous to boost the form of based-OOH* radical, then decrease the overpotential. Considering the particular simplicity of growing the Co2.1Mn0.9O4on graphite plates, this work is expected to provide a feasible way to develop the high-performance Co-Mn bimetallic oxide for water splitting.Keywords:water splitting;bimetallic oxides;Mn-doped Co3O4;DFT calculation
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
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IF 22.1
Huiling Zhang,Xiaomei Zhou,Longxin Liu,Fujun Lan,Teng Zhao,Mo Qiu,Qingxin Guan,Wei Li
Atomically dispersed cluster catalysts own versatile applications in biomass valorization, while the controllable assembly and microenvironmental regulation remain a crucial challenge. Herein, Co clusters assembled via nanosized ZIF-67 sprouted from Co-Al layered double hydroxide nanoflowers were applied for selective hydrogenation of furfural (FAL). The pyrolysis temperature can tune the microstructures and acid properties of the catalyst, which accounts for the hydrogenation of FAL to furfuryl alcohol (FOL), 2-methylfuran (2-MF), and tetrahydrofurfuryl alcohol (THFOL) with yield of 99.1 %, 96.7 %, and 82.3 %, respectively. The Co clusters favor C O bond adsorption via bridging-type adsorption mode while suppressing the furan ring adsorption. Moreover, ultra-dispersed Co clusters facilitate the cleavage of C-OH bonds in FOL intermediate, leading to a high 2-MF yield. As the pyrolysis temperature increase, the formed Co nanoparticles are conducive to the parallel adsorption of FAL, resulting in the production of THFOL. This work affords a multi-functional catalyst in catalytic biomass upgrading.
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JOURNAL OF MEMBRANE SCIENCE
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2023
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IF 9.5
Xiang Qin,Xiaoping Feng,Dongying Hu
The asymmetric structures constructed via traditional methods fundamentally determine the “trade-off” bottleneck of cellulose triacetate reverse osmosis (RO) membrane in desalination. So, based on the structure-determined performance, inspired by the pore mechanism of frozen tofu through “water-ice-water” phase transition, the biomimetic RO membrane with high symmetry and homogeneity was successfully utilized in desalination. The co-solubilized N-methyl-2-pyrrolidone (NMP) narrowed the structural differentiation between Top and Bottom, increasing the number of through-water channels, surface hydrophilicity, and flatness of RO membrane. Typically, the prepared membrane with 0.125% NMP concentration has a salt rejection rate of 98.9% for NaCl, and excellent retention rate for other inorganic salts (MgCl 2 , LiCl). Notably, the NMP-modified membrane has a water flux of up to 17.2 L m −2 h −1 , which is nearly 660% higher than that of No porogen-RO membrane (2.6 L m −2 h −1 ). Further, the membrane retained its separation capacity even after continued operation for 700 min, owing to the enhanced compression of the ductile pores by NMP. Overall, this novel cellulose-based RO membrane represents a structural mechanism for the design of innovative biomimetic multi-channel structures for long-term and efficient desalination.
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