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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Curvature Effect of Pyridinic N-Modified Carbon Atom Sites for Electrocatalyzing CO2 Conversion to CO

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.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Fe0Ni0 bimetal co-immobilized horseradish peroxidase on ZIF-8@HMON for degradation of trichloroacetic acid

Yuxiang Yang,Xiaocui Huang,Mengyang Dong,Ziling Chang,Hongming Yuan,Yan Huang,Xiangnong Liu,Jianbo Zhang,Anbang Dai

As a common pollutant in the environment, trichloroacetic acid (TCA) is difficult to be completely degraded by common advanced oxidation processes (AOPs) due to its high C-Cl bond content. Advanced oxidation–reduction processes (AORPs) may improve the degradation performance of TCA. In this work, we use Fe 0 Ni 0 bimetal as reducing catalyst, hollow mesoporous silicone nanoparticles (HMONs) modified by ZIF-8 as immobilized carrier, horseradish peroxidase (HRP) and Fe 0 Ni 0 were fixed in the carrier to form a AORP system for degradation of TCA. The effects of temperature, pH, H 2 O 2 concentration, doping ratio on the degradation performance of the catalyst and the degradation mechanism of the composite catalyst were investigated. Degradation experiments showed that H· and OH· were present in the dual system, dechlorination and decarboxylation exist at the same time. Under the condition of 55 °C and pH = 4, 30 mg Fe 0 Ni 0 and 20 mg immobilized enzyme shows the best degradation on TCA, and 81.48 % of 20 mg·L −1 TCA could be degraded by 2 h.

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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2023 · IF 8.2

Supermolecular nanovehicles co-delivering TLR7/8-agonist and anti-CD47 siRNA for enhanced tumor immunotherapy

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.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Biomedical Optics Express · 2023 ·Vol. 15 ·期 1 ·306-318 · IF 3.4

Plasmon enhanced luminescence of Tb/Eu co-doped film by Au NRs-PVA nanocomposite film

Lianyu Zhang,Jinhua Liu,Linlin Tian,Dong Zhang,Dong Zhang,Qingru Wang

Plasmonic nanostructures have great potential for improving the radiation properties of emitters. Here, the plasmonic Au nanorods-PVA nanocomposite films are used to uniformly improve the photoluminescence of Tb/Eu co-doped PMMA film within the local micro-region. Under the excitation of 292 nm, the maximum enhancement factor is 37.2-fold for emission at 612 nm and 21.6-fold for emission at 545 nm. Moreover, the finite different time domain simulations are developed to further explain the experimental results. It is indicated that the modulation of luminescence can be attributed to the increase of the local density of optical states through the Purcell effect and the improvement of the energy transfer efficiency between Tb and Eu. Under the excitation of 360 nm, the maximum enhancement factor is about 71.5-fold. In this case, the Au nanorods are mainly used for modulating the emission process at 612 nm, which deduced a greater enhancement factor at 612 nm. This study provides a deep understanding of the interactions between rare earth ions co-doped materials and plasmonic nanostructures, building a bridge to fabricate a useful platform for several applications, such as thin film-based detectors and sensors.

CAS / MDL: 15492-51-0
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

From asymmetry to symmetry: Biomimetic multi-channel structures for enhanced desalination using co-dissolving porogens

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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Batteries-Basel · 2023 ·Vol. 9 ·期 7 ·352 · IF 4

Anion and Cation Co-Modified Vanadium Oxide for Cathode Material of Aqueous Zinc-Ion Battery

Xueqi Zhang,Ruilin Bian,Zhiyuan Sang,Shandong Tan,Ji Liang,Liqun Wang,Feng Hou

Aqueous zinc-ion batteries (ZIBs) have been regarded as a promising alternative to traditional lithium-based batteries due to their intrinsic advantages of safety, low cost, and abundance. However, the strong electrostatic interaction between Zn2+and the layer-structured cathodes is still a key issue that hinders the batteries from storing more Zn. Herein, we report partially nitrided and cation-doped vanadium oxide for improved Zn storage performance. Specifically, the defects and nitride species that are generated inside the material upon nitriding improve the conductivity of the material and introduce a new Zn storage mechanism. The intercalation of cations, in contrast, widens the interlayer spacing to store more Zn2+ions and enhances the cycling stability of the material. These merits synergistically lead to significantly enhanced electrochemical Zn2+ion storage performance, in terms of a high specific capacity of 418.5 mAh·g−1at a current density of 0.1 A·g−1and a capacity retention of 81.2% after 500 cycles at 2.0 A·g−1. The new modification strategy for V2O5suggested in this work could provide insight into the development of high-performance ZIBs.Keywords:aqueous zinc-ion batteries;cathode materials;vanadium oxide;partial nitridation;anion/cation co-doping

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COLLOID AND POLYMER SCIENCE · 2023 ·Vol. 301 ·期 8 ·957-966 · IF 2.4

Facile fabrication of superhydrophilic poly(styrene-co-acrylate)/SiO2 composite materials by conventional emulsion polymerization

Liao Wenbo,Wu Weicai,Zhong Guoyu,Ye Lingyun,Zheng Shaona

A novel procedure for the preparation of superhydrophilic poly(styrene-co-acrylate)/SiO 2 composite materials was prepared from conventional emulsion polymerization in the presence of colloidal silica. TEM photos revealed that poly(styrene-co-acrylate) latexes exhibited a clear core–shell structure, and the electrostatic repulsion and hydrogen bonds between poly(styrene-co-acrylate) latexes and SiO 2 nanoparticles guaranteed the uniform dispersion of silica nanoparticles. The average diameter data indicated that the particle size of composite latexes (78 nm) was slightly smaller than that of polymer (82 nm), although the slight aggregation of SiO 2 nanoparticles had increased the average diameter to 87 nm. FTIR spectra confirmed that hydrogen bonds were formed and gel reaction of –OH groups occurred during film formation. Two kinds of Si–O bonds were found in XPS spectra with a weight ratio addition of 20.0% SiO 2 , which one was related to the Si–OH groups of colloidal silica nanoparticles, while the other was attributed to the Si–O-Si groups obtained from the gel reaction. SEM and AFM images displayed that the formation of micro/nano structure from the gel reaction had increased the roughness of the composite films. The water contact angle (WCA) of the composite films was found to decrease from 45 to 3º (3 s) and exhibit superhydrophilicity. Graphical abstract

CAS / MDL: 27813-02-1 9086-85-5
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Nature Communications · 2023 ·Vol. 14 ·期 1 ·1-14 · IF 16.6

Exploiting synergistic effect of CO/NO gases for soft tissue transplantation using a hydrogel patch

Tang Xiaoduo,Ren Jingyan,Wei Xin,Wang Tao,Li Haiqiu,Sun Yihan,Liu Yang,Chi Mingli,Zhu Shoujun,Lu Laijin,Zhang Junhu,Yang Bai

Autologous skin flap transplantation is a common method for repairing complex soft tissue defects caused by cancer, trauma, and congenital malformations. Limited blood supply range and post-transplantation ischemia-reperfusion injury can lead to distal necrosis of the flap and long-term functional loss, which severely restricts the decision-making regarding the optimal surgical plan. To address this issue, we develop a hydrogel patch that releases carbon monoxide and nitric oxide gases on demand, to afford a timely blood supply for skin flap transplantation during surgery. Using an ischemia-reperfusion dorsal skin flap model in rats, we show that the hydrogel patch maintains the immediate opening of blood flow channels in transplanted tissue and effective blood perfusion throughout the perioperative period, activating perfusion of the hemodynamic donor site. We demonstrate that the hydrogel patch promotes distal vascularization and long-term functional reconstruction of transplanted tissues by inhibiting inflammatory damage and accelerating blood vessel formation.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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International Journal of Electrochemical Science · 2023 · IF 1.5

Highly Active Pt-Co/C Nanoparticles: Controllable Preparation and Catalytic Performance for Methanol Electro-oxidation

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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ELECTROCHIMICA ACTA · 2023 · IF 6.6

Tuning the electronic configuration of Co-Nx for highly efficient H2O2 production in acidic solution

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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Journal of Materials Chemistry B · 2023 ·Vol. 11 ·期 26 ·6147-6158 · IF 7

Immunological gadolinium-doped mesoporous carbon nanoparticles for tumor-targeted MRI and photothermal-immune co-therapy

Xiaoxi Song,Chun Zhang,Mengyuan Xing,Chunyan He,Dongxu Wang,Lijuan Chong,Xiuli Zhang,Minghui Chen,Jingjing Li

Photothermal therapy (PTT) is an effective and well-documented approach to thermally ablate tumors. However, the side effect of distal metastasis and recurrence limit its further expansion. At the same time as PTT was developed, the employment of imaging to monitor the treatment of tumors also became meaningful. Herein, as a proof of concept, gadolinium-doped mesoporous carbon nanoparticles (Gd-MCNs) were prepared as nanocarriers, MRI contrast agents, and PTT agents by a one-step hard template method, which realized Gd doping and carbon filling simultaneously, while retaining enough pore space for drug loading. After loading the immune adjuvant, R837, and the coating of tumor extracellular vesicle, the obtained biomimetic nanoparticles (EV@Gd-MCNs-R837) not only allowed tumor MRI, but also inhibited the primary tumor and its metastasis with long-term immune memory in vivo. This study provides proof for the potential of Gd-MCNs-based biomimetic nanoparticles for targeted PTT/immune-enhanced synergistic theranostic of tumors.

CAS / MDL: 111-41-1 57-09-0
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INDUSTRIAL CROPS AND PRODUCTS · 2023 · IF 5.9

Catalytic co-pyrolysis of cellulose over alkali and alkaline earth metal salts for levoglucosan production

Miao Wang,Shuai Zhang,Xiangjun Liu,Yayun Ma,Junqi Wang

A comprehensive study of alkali and alkaline earth metal (AAEM) salts including two different anions (Cl - and CH 3 COO - ) in the catalytic pyrolysis of cellulose to produce levoglucosan (LG), bio-oil, and biochar were investigated. At the same time, the catalytic pyrolysis mechanism was also speculated. The thermogravimetric analyzer (TGA) and lab-scale fixed-bed reactor system were used to determine the thermal degradation process and the pyrolysis products of LG, bio-oil, and biochar. The optimized pyrolysis parameters were obtained by using Box-Behnken design-response surface method. According to the results, AAEM salts significantly boosted the yield of biochar, as well as greatly cut down the output of LG and bio-oil. The rank of effect on LG yield was as follows: CaCl 2 , MgCl 2 > CH 3 COOK, CH 3 COONa > (CH 3 COO) 2 Mg, (CH 3 COO) 2 Ca > KCl, NaCl. Moreover, the addition of AAEM salts considerably dropped the activation energy E of cellulose pyrolysis as well as prompted microcrystalline cellulose pyrolysis under lower temperatures. This study was pivotal in deducing the pathway of cellulose pyrolysis, thereby offering critical insights to hasten the progress of biomass utilization.

CAS / MDL: 9004-34-6
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