JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Tiantian Feng,Zhijie Cui,Pengfei Guo,Xuehong Wang,Juan Li,Xien Liu,Wenpin Wang,Zhongcheng Li
Recent experimental analysis indicates WO 3 -based nanostructures exhibit poor hydrogen evolution reactivity, particularly in alkaline medium, arising from the low electron transfer rate. It is imperative to tune the composition and structure of WO 3 to boost the cleavage of H-OH bond. Here, we construct Ru/WO 3 -W 2 N/N-doped carbon sheets (Ru/WO 3 -W 2 N/NC) using m-WO 3 nanosheets as precursors with the aid of RuCl 3 , Tris (hydroxymethyl) aminomethane, and dopamine. Structural investigation reveals the formation of N-doped carbon sheets, Ru nanoparticles, and WO 3 -W 2 N. As a result, hydrogen evolution reactivity is greatly improved on Ru/WO 3 -W 2 N/N-doped carbon sheets with 64 mV at 10 mA/cm 2 in 1 mol/L (M) KOH, outperforming most of WO 3 -based electrocatalysts in previous literatures. Meanwhile, it facilitates the generation of H 2 in 0.5 M H 2 SO 4 with the excellent activity of 110 mV at 10 mA/cm 2 . Our work provides an efficient strategy to tailor the electronic structure of WO 3 to catalyze acidic and alkaline hydrogen evolution reaction.
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Guodong Sun,Yanan Cao,Deqing Li,Mingzhen Hu,Xinhu Liang,Zhe Wang,Zengjian Cai,Fengyi Shen,Bozhen Chen,Kebin Zhou
Electrochemical reduction of CO 2 to multi-carbon products is very attractive yet particularly challenging due to the low efficiency of C-C coupling over currently used electrocatalysts. In this work, we report a dual-atom catalyst (Cu 2 /NC) capable of selectively promoting electro-reduction of CO 2 to C 2 H 4 . The Faradaic efficiency of CO 2 -to-C 2 H 4 over the Cu 2 /NC is up to ∼34.9% with a current density of 33.6 mA·cm −2 . By contrast, its Cu single-atom counterpart only generates CO without forming C 2 H 4 . The density functional theory (DFT) calculations reveal that the Cu-Cu sites largely promote the adsorption of *CO and reduce the energy barrier of C-C coupling between the adsorbed *CO relative to that of the single Cu sites, which accounts for the high C 2 H 4 selectivity of the Cu 2 /NC.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jiangna Xing,Xin Huang,Xin Yong,Xin Li,Jun Li,Jingkang Wang,Na Wang,Hongxun Hao
Metal-free g-C 3 N 4 has received wide attentions because of the economy and environmental friendliness of it. However, the synthesis of simple and efficient g-C 3 N 4 modified materials is still challenging. In this study, series of novel N -doped porous thin-walled g-C 3 N 4 nanotubes (CNx) were synthesized through supramolecular self-assembly and thermal polymerization using melamine and aminourea hydrochloride as raw materials. SEM, XRD, XPS, etc. were used to analyze microscopic morphology and chemical structure of synthesized photocatalysts. PL spectra, EIS Nyquist curves and UV–vis DRS, etc. were applied to study the photoelectrochemical and optical properties. Besides, the performance of the synthesized catalysts was illustrated through TC photodegradation experiments, and the degradation rate of tetracycline (TC) by CN0.75 can reach to 93.0 % and the reaction rate constant was calculated to be 0.1347 min −1 . The excellent photocatalytic activity is primarily related to higher specific surface area and the formation of midgap states after N doped, which is conducive to the separation of charges. Finally, the possible pathways and mechanisms were proposed by determining the degradation intermediates and active species in the TC photodegradation process.
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ACS Applied Energy Materials
·
2023
·
IF 6.4
Jinghong Chen,Wei Yuan,Yaopeng Wu,Xiaoqing Zhang,Simin Jiang,Bote Zhao,Yu Chen,Chenghao Yang,Liangxin Ding,Yong Tang,Xinrui Ding
Motivated by the advancements in portable and wearable electronics, the rising necessity for microscale energy storage electronics has prompted extensive research on the efficient and cost-effective preparation of high-performance electrode materials. Herein, a facile fabrication method of N-doped graphene-based electrodes is demonstrated for in-plane microsupercapacitors (MSCs) on flexible textile. Our approach involves a one-step direct hot stamping of 10 s for efficient reduction of graphene oxide (GO) and simultaneously N doping into reduced GO (N-rGO). The degree of N doping is controlled by varying the concentrations of precursor chitosan (CS) in GO. Benefiting from the enhanced N doping, the N-rGO 15% electrodes prepared with a CS-to-GO mass ratio of 0.15 exhibit excellent volumetric capacitance of 42.2 F cm–3, exceptional energy density of 3.01 mWh cm–3, and a maximum power density of 31.57 mW cm–3, along with the outstanding mechanical flexibility and cycle stability. Besides, serial integration of the MSCs interwoven on short sleeves was also performed to light a customized LED, suggesting its potential as a power source in wearable devices. Therefore, the proposed hot stamping strategy offers insights for the development of an integrated and multifunctional textile.
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MRS Communications
·
2023
·Vol. 13
·期 4
·538-545
·
IF 1.9
Yin Jinkun,Chu Yaoqing,Tan Lianjiang
Cu/N co-doped TiO 2 nanopowder was prepared with a facile sol–gel method. In the absence of stabilizing agents, the co-doped nanopowder with nanoscaled particle sizes was obtained. Doping didn’t change the anatase crystal structure of TiO 2 . Cuprite Cu 2 Cl(OH) 3 formed in the co-doped nanopowder. Based on ultraviolet–visible (UV–vis) spectroscopy and X-ray photoelectron spectroscopy (XPS) data, the mechanisms of significantly improved photocatalytic activity of the co-doped nanopowder were discussed. The antibacterial evaluation and cytotoxicity test suggested the nanopowder inhibited bacteria significantly under visible light and had ultralow cytotoxicity. This work provided a promising antibacterial agent with potential biomedical applications.
Graphical abstract
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Frontiers in Bioengineering and Biotechnology
·
2023
·
IF 5.7
Qian Zhang,Xingyuan Qu,Chen Liang,Hongyan Li,Siyu Du,Chang Wang,Yuandong Xie,Yi Zheng,Lei Wang
Objective: This study aimed to investigate the regulatory effect of N-isopropylacrylamide-modified polyethyleneimine (PEN)-delivered oligodeoxynucleotide (ODN) MT01 on bone regeneration in vitro and in vivo . Methods: A polyethylenimine (PEI) derivative, PEN, was constructed through Michael addition and employed as a carrier for ODN MT01 transfection. PEN/MT01 nanocomposites were characterized using agarose gel retardation assay, size distribution, zeta potential and transmission electron microscopy. The Cell Counting Kit-8 (CCK-8) assay was used to detect the effect of PEN on cell viability. Alkaline phosphatase (ALP) staining was used to detect the osteogenic differentiation ability of PEN/MT01 nanocomposite. Real-time quantitative PCR (q RT-PCR) and enzyme-linked immunosorbent assay (ELISA) were used to detect the regulatory effects of PEN/MT01 nanocomposite on osteogenic differentiation gene expression. Rat model was observed using the skull defect method and verified using micro-computed tomography (CT), serum biochemical indices, hematoxylin and eosin (H&E) staining and Immunohistochemistry (IHC). Results: PEN had good biological properties and could deliver MT01 well to achieve efficient transmission of MT01. PEN/MT01 nanocomposites were effectively transfected into MC3T3-E1 cells at a ratio of 6.0. CCK-8 assay displayed that PEN had no cytotoxicity to MC3T3-E1 cells. Additionally, PEN/MT01 nanocomposites could promote the expression of osteogenic genes. In vivo results revealed that PEN/MT01 nanocomposites could promote bone regeneration more effectively than the other groups. Conclusion: PEN has good biocompatibility and low toxicity, which is a good carrier for ODN MT01. PEN-delivered MT01 can be potentially employed as a useful approach to achieving bone regeneration.
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Small
·
2022
·Vol. 18
·期 44
·2203976
·
IF 15.153
Anding Xu,Qi Zhu,Guilan Li,Caihong Gong,Xue Li,Huaming Chen,Jie Cui,Songping Wu,Zhiguang Xu,Yurong Yan
Metallic Bi, as an alloying-type anode material, has demonstrated tremendous potential for practical application of potassium-ion batteries. However, the giant volume expansion, severe structure pulverization, and sluggish dynamics of Bi-based materials result in unsatisfied rate performance and unstable cycling stability. Here, 2D bismuth@N-doped carbon sheets with Bi O C bond and internal void space (2D Bi@NOC) are successfully fabricated via a self-template strategy to address these issues, which own ultrafast electrochemical kinetics and impressive long-term cycling stability for delivering an admirable capacity of 341.7 mAh g −1 after 1000 cycles at 10 A g −1 and impressive rate capability of 220.6 mAh g −1 at 50 A g −1 . Particularly, the in situ transmission electron microscopy observations visualize the real-time alloying/dealloying process and reveal that plastic carbon shell and void space can availably relieve dramatic volume stress and powerfully maintain structural integrity. Density functional theory calculation and ultraviolet photoelectron spectroscopy test certify that the robust Bi O C bond is thermodynamically and kinetically beneficial for adsorption/diffusion of K + . This work will light on designing advanced high-performance energy materials and provide important evidence for understanding the energy storage mechanism of alloy-based materials.
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ACS Applied Energy Materials
·
2022
·
IF 6.959
Hongxia Liu,Shun Zhang,Yan Zhang,Shuotong Zong,Wang Li,Can Zhu,Feng Luo,Jian Wang,Zhigang Sun
SnSe is a promising medium-temperature thermoelectric material due to its extremely low thermal conductivity and tunable electronic transport properties. In this work, n-type SnSe0.95 polycrystals doped with CeCl3 are synthesized by a melting method combined with a spark plasma sintering (SPS) process. The samples have highly textured structures and anisotropic thermoelectric properties. CeCl3 doping has a favorable effect on the electronic transport above 473 K, which may benefit from the excitation of the introduced impurity energy level. Moreover, the thermal conductivity is significantly reduced due to the phonon scattering by point defects. Finally, a peak ZT value of 1.17 is obtained at 773 K in SnSe0.95–0.5 mol % CeCl3, which paves the way for improving the thermoelectric performance of n-type SnSe via rare-earth halide doping.
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ChemistrySelect
·
2022
·Vol. 7
·期 37
·e202200839
·
IF 2.307
Di Bai,Jipeng Meng,Chuang Li,Mingming Zhang,Changhai Liang
Graphical Alkali treatment and acid treatment were conducted on ZSM-23 zeolite, which achieved the acidity manipulation and improved the mesoporosity of the zeolite. The modification of the support was conducive to catalysts when used for n -hexadecane hydroisomerization, which enhanced the selectivity of isomers significantly and inhibited the cracking processes. The enhanced mesoporosity in the networks is expected to offer a potential route to surmount mass-transport constraints within one-dimensional microporous structural zeolites. Highly crystalized ZSM-23 zeolite was synthesized and subsequently post-treated with alkali-etching and acid-etching, the effects of post-treatments on the physical and chemical properties of the parent zeolite were investigated via XRD, N 2 physical adsorption, FE-SEM, TEM, 27 Al MAS NMR, Py-IR and NH 3 -TPD. The catalytic activity of various Pt supported bifunctional catalysts was investigated via n -hexadecane hydroisomerization. The post-treated process not only increased the pore volume as well as the specific surface area, which efficiently improved the diffusion efficiency, but also changed the acidity and acid distribution of zeolite: alkali treatment could increase the content of total Brönsted acid while acid treatment exhibited an opposite trend. Acid treatment effectively promoted the density of weak Brönsted acid sites and suppressed the med-strong Brönsted acid sites. With the manipulation of acidity and development of mesoporosity in zeolite, the formation of isomers and the suppression of cracked products in the n -hexadecane hydroisomerization were accomplished. The catalytic performance of catalysts showed that acid treatment could effectually promote the formation of isomeric products and inhibit cracking reactions. Especially, Pt/Z(1.0 HN) catalyst with suitable distribution of acid sites and textural properties, exhibited an outstanding n -C 16 hydroisomerization performance with the highest i -C 16 yield of 64 wt.% at 340 °C.
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Journal of the American Chemical Society
·
2022
·
IF 16.383
Fei Xiao,Yian Wang,Gui-Liang Xu,Fei Yang,Shangqian Zhu,Cheng-Jun Sun,Yingdan Cui,Zhiwen Xu,Qinglan Zhao,Juhee Jang,Xiaoyi Qiu,Ershuai Liu,Walter S. Drisdell,Zidong Wei,Meng Gu,Khalil Amine,Minhua Shao
The poor durability of Pt-based nanoparticles dispersed on carbon black is the challenge for the application of long-life polymer electrolyte fuel cells. Recent work suggests that Fe- and N-codoped carbon (Fe–N–C) might be a better support than conventional high-surface-area carbon. In this work, we find that the electrochemical surface area retention of Pt/Fe–N–C is much better than that of commercial Pt/C during potential cycling in both acidic and basic media. In situ inductively coupled plasma mass spectrometry studies indicate that the Pt dissolution rate of Pt/Fe–N–C is 3 times smaller than that of Pt/C during cycling. Density functional theory calculations further illustrate that the Fe–N–C substrate can provide strong and stable support to the Pt nanoparticles and alleviate the oxide formation by adjusting the electronic structure. The strong metal–substrate interaction, together with a lower metal dissolution rate and highly stable support, may be the reason for the significantly enhanced stability of Pt/Fe–N–C. This finding highlights the importance of carbon support selection to achieve a more durable Pt-based electrocatalyst for fuel cells.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Le Wang,Pengyu Niu,Hongjuan Xi,Xiaoyan Chen,Congbiao Chen,Zhongyi Ma,Litao Jia,Bo Hou,Debao Li
The ZSM-22/ASA composite material for efficient hydroisomerization of n-dodecane was successfully prepared via a two-step synthesis method. The structure, pore properties, and acidity of the catalysts were elucidated by the means of XRD , N 2 physical adsorption, TEM, FT-IR, and Py-IR. Compared with the mixture catalyst, ZSM-22/ASA has a higher average pore diameter and formed a uniform and open channel structure, which is favorable to the diffusion of the reactant and the efficiency of the acid sites. The zeolite and the ASA phase in the composite are closely bonded by the interface effect, forming an additional Si–O–Al structure, which significantly affected the acidity of the composite catalyst. ZSM-22/ASA composite material exhibits enhanced n-dodecane hydroisomerization selectivity of total isomers and multi-branched isomers, which is attributed to its proper acid strength and pore structure conducive to diffusion. Finally, the location distribution of branched methyl groups was discussed and enhanced more central branching iso-dodecanes was obtained over the ZSM-22/ASA composite material.
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ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 38
·2202675
·
IF 19.924
Mingzhen Hu,Zengjian Cai,Xinhu Liang,Ganggang Li,Haiyan Tan,Shitu Yang,Hao Ren,Zhe Wang,Guodong Sun,Shoujie Liu,Zhengping Hao,Kebin Zhou
It is extremely challenging to controllably synthesize rare earth-containing nanoalloys due to the ultralow standard reduction potential of rare earth metals. Here, a surface-confined strategy to prepare ultrafine Pt-rare earth nanoalloys on a series of N-functionalized supports is reported. It proves that by surface N-metal coordination, the metal cations of precursors are atomically dispersed on support, which greatly favors uniform nucleation and growth of particles upon reduction. Moreover, the moderate metal transfer barrier from N ensures particle growth in a confined region to form ultrafine nanoalloys. Using this method, ultrafine Pt La, Pt Y, and Pt Dy nanoalloys are prepared on N-functionalized supports such as carbon, zeolite, and Al 2 O 3 . Notably, the Pt La nanoalloys on N-functionalized zeolite show superior activity and durability for propane oxidation. The strategy is expected to provide guidelines for preparing highly efficient rare earth-containing nanoalloys for catalysis applications.
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