ADVANCED MATERIALS
·
2020
·Vol. 32
·期 39
·2002382
·
IF 27.398
Changming Zhao,Gan Luo,Xiaokang Liu,Wei Zhang,Zhijun Li,Qian Xu,Qinghua Zhang,Huijuan Wang,Deming Li,Fangyao Zhou,Yunteng Qu,Xiao Han,Zezhou Zhu,Geng Wu,Jing Wang,Junfa Zhu,Tao Yao,Yafei Li,Henny J.M. Bouwmeester,Yuen Wu
Electrochemical reduction of CO to value-added products holds promise for storage of energy from renewable sources. Copper can convert CO into multi-carbon (C 2+ ) products during CO electroreduction. However, developing a Cu electrocatalyst with a high selectivity for CO reduction and desirable production rates for C 2+ products remains challenging. Herein, highly lattice-disordered Cu 3 N with abundant twin structures as a precursor electrocatalyst is examined for CO reduction. Through in situ activation during the CO reduction reaction (CORR) and concomitant release of nitrogen, the obtained metallic Cu° catalyst particles inherit the lattice dislocations present in the parent Cu 3 N lattice. The de-nitrified catalyst delivers an unprecedented C 2+ Faradaic efficiency of over 90% at a current density of 727 mA cm −2 in a flow cell system. Using a membrane electrode assembly (MEA) electrolyzer with a solid-state electrolyte (SSE), a 17.4 vol% ethylene stream and liquid streams with concentration of 1.45 m and 230 × 10 −3 m C 2+ products at the outlet of the cathode and SSE-containment layer are obtained.
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Advanced Energy Materials
·
2024
·
IF 24.4
Gaojing Yang,Yaxun Zhu,Zhimeng Hao,Qiu Zhang,Yong Lu,Zhenhua Yan,Jun Chen
Redox flow batteries (RFBs) are considered as promising candidates for large-scale energy storage. However, traditional RFBs based on toxic metal ions have deficiencies in resource utilization and environmental protection. Considering the corrosiveness of acidic and alkaline electrolytes and sustainability of energy storage devices, neutral aqueous organic redox flow batteries (AORFBs) have more development prospects. Herein, an AORFB is reported, using 9,10-anthraquinone-2,7-disulfonic salt (2,7-AQDS) and 1,4-dihydroxyphenylsulfonate potassium (HQS) as negative and positive electroactive materials, respectively. It is found that the anions in the neutral solution further affected the solubility and kinetics of the electroactive materials by affecting the hydrogen bond in the solution, and the Na 2 SO 4 solution showed the optimal comprehensive performance. Therefore, an all-quinone AORFB employing neutral Na 2 SO 4 electrolytes with a cell voltage of 0.9 V is constructed, which presented a capacity utilization of 70.1% and delivered stable cycling performance at 60 mA cm −2 . This work designs an innovative neutral all-quinone AORFB and points out how anions affect the properties of the electrolyte by affecting hydrogen bonds within the solution. These findings open a new avenue for the design and application of neutral all-organic aqueous RFBs.
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SusMat
·
2025
·
IF 21.3
Xuechun Hu,Yuchen Pang,Chaoqun Li,Xiaoyue Zhang,Xuebin Yu,Fang Fang,Guanglin Xia
Magnesium hydride (MgH 2 ) has been regarded as an attractive candidate for solid-state hydrogen storage, yet its practical applications are limited by the requirement of elevated temperatures and sluggish hydrogen uptake and release kinetics. Herein, TiO 2 polyhedral frameworks with uniformly distributed V 2 O 5 (denoted as V 2 O 5 /TiO 2 ) are constructed to improve hydrogen storage performance of Mg/MgH 2 . During the reversible hydrogenation and dehydrogenation process, metallic V and Ti along with low-valent Ti- and V-based oxides are in situ formed. Among them, metallic V supported on TiO 2 exhibits the lowest hydrogen adsorption energy, enabling superior catalytic performance over TiO 2 and V 2 O 5 . As a result, the peak dehydrogenation temperature of MgH 2 decreases to 215°C, 105°C lower than that of pristine MgH 2 , with a decrease of the apparent activation energy from 139.50 kJ·mol −1 to 68.99 kJ·mol −1 . Moreover, electron migration from V toward TiO 2 leads to charge accumulation around Ti and O atoms, shifting the V 3 d -band center toward the Fermi level and thereby improving the catalytic function of V's d-electrons, facilitating hydrogen dissociation without energy barriers. Therefore, the V 2 O 5 /TiO 2 -catalyzed Mg absorbs 4.12 wt% H 2 under an ultralow pressure of 1 bar at 25°C. This provides a new strategy for developing advanced Ti and V-based catalysts for mild-condition hydrogen storage of MgH 2 .
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CELL
·
2025
·
IF 42.5
Xing Guo,Yichuan Wang,Caiyao Zhao,Cong Tan,Wei Yan,Sunhuan Xiang,Dan Zhang,Hui Zhang,Mengting Zhang,Liujing Yang,Meng Yan,Pingli Xie,Yi Wang,Li Li,Dongming Fang,Xuanmin Guang,Wenwen Shao,Fang Wang,Haoxuan Wang,Sunil Kumar Sahu,Min Liu,Tong Wei,Yang Peng,Yuping Qiu,Tao Peng,Yi Zhang,Xuemei Ni,Zhicheng Xu,Haorong Lu,Zhonghai Li,Huanming Yang,Ertao Wang,Michael Lisby,Huan Liu,Hongwei Guo,Xun Xu
With rapid advancements in single-cell RNA sequencing (scRNA-seq) technologies, exploration of the systemic coordination of critical physiological processes has entered a new era. Here, we generated a comprehensive Arabidopsis single-nucleus transcriptomic atlas using over 1 million nuclei from 20 tissues encompassing multiple developmental stages. Our analyses identified cell types that have not been characterized in previous single-protoplast studies and revealed cell-type conservation and specificity across different organs. Through time-resolved sampling, we revealed highly coordinated onset and progression of senescence among the major leaf cell types. We originally formulated two molecular indexes to quantify the aging state of leaf cells at single-cell resolution. Additionally, facilitated by weighted gene co-expression network analysis, we identified hundreds of promising hub genes that may integratively regulate leaf senescence. Inspired by the functional validation of identified hub genes, we built a systemic scenario of carbon and nitrogen allocation among different cell types from source leaves to sink organs.
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CEMENT AND CONCRETE RESEARCH
·
2016
·
IF 3.48
Zuhua Zhang,John L. Provis,Jin Zou,Andrew Reid,Hao Wang
Variations between fly ashes can lead to significant differences in the geopolymers derived from them, in both microstructural and mechanical properties. This study assesses the effect of physical, crystallographic and chemical characteristics of fly ash on geopolymerisation performance and the strength of the resulting binders. Physical and glass chemistry factors are combined to develop a comprehensive index to evaluate the suitability of fly ashes for the production of high-strength geopolymers. An equation for this index is proposed, developed using five typical low-calcium fly ashes and then validated against a further eight literature datasets, showing a good relationship between the ranking order of the calculated index and the compressive strengths of geopolymer pastes produced with comparable activator and paste workability. This index can be used to screen the source materials, which is of significant value in moving alkali activated cements towards acceptance in practice.
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COMPOSITES SCIENCE AND TECHNOLOGY
·
2018
·
IF 5.16
Weiqiang Zhi,Shanglin Xiang,Renji Bian,Ruizhi Lin,Kaihua Wu,Tingwei Wang,Dongyu Cai
In this work, an emulsion method is applied to fill two-dimensional MXenes into polyurethanes (PUs). It shows that the addition of 0.5 wt% MXenes increase the yield stress, tensile strength and hardness of PUs by ∼70%, ∼20% and ∼13%, respectively. The mechanical enhancement is associated with the increase of hardness and reduction of water absorption. Morphologic study shows that a good dispersion of MXenes is achieved, in which ball milling is a key step for ensuring a stability of MXene-filled PU emulsions. Furthermore, FTIR analysis reveals the strong interaction between MXenes and PUs at molecular level.
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ELECTROCHIMICA ACTA
·
2014
·
IF 4.086
Tian Xu,Guangjin Wang,Cong Liang,Mu Pan
Nitrogen shows a positive influence on the ORR activity of certain catalysts, such as N-doped carbon and N-doped ZrO 2 . In this paper, we report a method to dope nitrogen into La 2 Zr 2 O 7 nanoparticles by the sol-gel process combined with ammonolysis. XPS results indicate that the nitrogen content in La 2 Zr 2 O 7 is approximately 0.92 at.%. Compared to the ORR activity of La 2 Zr 2 O 7 , ORR activity of the N-doped La 2 Zr 2 O 7 is considerably enhanced. Density functional theory (DFT) calculations indicate that the band gap is reduced in N-doped La 2 Zr 2 O 7 , which may be one of the factors that contribute to the improvement.
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JOURNAL OF MATERIALS ENGINEERING AND PERFORMANCE
·
2023
·Vol. 33
·期 20
·11309-11320
·
IF 2.3
Zhang Dongbo,Feng Xiaolong,Song Ruiqing,Wang Ning,Zhang Yongsheng
Thermal barrier coating (TBC) is applied to protect the hot-section components of a gas turbine engine. In the present work, a La 2 (Zr 0.2 Ti 0.2 Y 0.2 YB 0.2 Nb 0.2 ) 2 O 7 high entropy oxide was designed, fabricated by a solid-phase reaction at 1400 °C, and subjected to an investigation of its properties. The results indicate that the La 2 (Zr 0.2 Ti 0.2 Yb 0.2 Y 0.2 Nb 0.2 ) 2 O 7 high entropy oxide had a pyrochlore structure. During synthesis, a small amount of La 2 TiO 5 was produced. The thermal conductivity of the La 2 (Zr 0.2 Ti 0.2 Yb 0.2 Y 0.2 Nb 0.2 ) 2 O 7 high entropy oxide was approximately 0.8855 W·m -1 ·K -1 at room temperature. The coefficient of thermal expansion of the La 2 (Zr 0.2 Ti 0.2 Yb 0.2 Y 0.2 Nb 0.2 ) 2 O 7 high entropy oxide was approximately 9.374 × 10 −6 K −1 at 1000 °C. To improve the service life of the TBC composed of the La 2 (Zr 0.2 Ti 0.2 Yb 0.2 Y 0.2 Nb 0.2 ) 2 O 7 , a double-layer structural coating composed of La 2 (Zr 0.2 Ti 0.2 Y 0.2 YB 0.2 Nb 0.2 ) 2 O 7 and yttria-stabilized zirconia (YSZ) layers was designed and produced on a NiCoCrAlY alloy by laser cladding. The thermal cycling behavior of the double-layer coating was studied at 1050 °C. The results indicate that a La 2 (Zr 0.2 Ti 0.2 Yb 0.2 Y 0.2 Nb 0.2 ) 2 O 7 single-phase defective-fluorite high entropy oxide was produced after preparation and thermal cycling. The spallation of the double-layer coating composed of La 2 (Zr 0.2 Ti 0.2 Yb 0.2 Y 0.2 Nb 0.2 ) 2 O 7 /YSZ occurred after 70 thermal cycles at 1050 °C. The double-layer coating composed of La 2 (Zr 0.2 Ti 0.2 Yb 0.2 Y 0.2 Nb 0.2 ) 2 O 7 /YSZ can increase the thermal cycling lifetime of TBCs containing high entropy oxides.
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INORGANIC CHEMISTRY
·
2026
·
IF 4.6
Lin Wei,Yang Zhibin,Tao Jin-Gang-Lu,Zhao Qianqian,Liu Fuyu,Li Wanshan,Feng Renfei,Zhang Yu,Fu Xian-Zhu,Luo Jing-Li,Zhao Bin
Developing efficient and durable electrocatalysts for
alkaline
seawater hydrogen evolution remains challenging because of sluggish
water dissociation kinetics. Herein, we report a defect-rich d-p orbital-hybridized
Os/o-CNTs electrocatalyst ( dph -Os def /o-CNTs)
prepared by rapid room-temperature NaBH 4 reduction. The
partially oxidized CNT support anchors defective Os nanoclusters and
induces C–Os/C–O–Os electronic coupling, generating
electron-deficient Os sites with modulated 5d electronic structures.
In alkaline simulated seawater (1 M NaOH + 3.5 wt % NaCl), dph -Os def /o-CNTs requires only 91 mV to reach
100 mA cm –2 and exhibits a Tafel slope of 19 mV
dec –1 , with stable operation over 350 h and 10,000
CV cycles. In situ Raman spectroscopy, AIMD simulations, and DFT calculations
reveal that Os vacancies reorganize interfacial water into an ordered
H-bond network, promote O-down water adsorption, and reduce the water
dissociation barrier from 1.12 to 0.56 eV. Moreover, an Al | OH – | H 2 primary cell using dph -Os def /o-CNTs as the cathode delivers 1.41 V and 10.92
mW cm –2 , enabling simultaneous hydrogen generation
and electricity output.
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ACS Applied Bio Materials
·
2020
·
IF 0
Chang Liu,Xinrui You,Dingkun Lu,Guoyue Shi,Jingjing Deng,Tianshu Zhou
Nowadays, the environmental risk factors for Alzheimer’s disease (AD) have received widespread attention. Two major amyloid-β peptide (Aβ) variants, Aβ42 and Aβ40, play a pivotal role in the etiology of AD and the concentration ratio of which (i.e., Aβ42%) has been suggested to be the superior biomarker for AD. In this study, an “aggregation-based colorimetric sensor array” for the simultaneous identification and detection of Aβ40 and Aβ42 with structural similarity was established based on gelsolin-modified silver nanotriangles (Ag NTs) and silver nanorods (Ag NRs). Different aggregation behaviors of gelsolin-modified Ag NTs and Ag NRs in the presence of Aβ42 and Aβ40 resulted in different color and spectral changes, which could be quantitatively analyzed in terms of unique spectral patterns by principal component analysis. With the colorimetric sensor array employed here, the fluctuation of Aβ42% in different brain regions of rats exposed to Cd2+ could be directly monitored. The downward trend of Aβ42% accompanied by variations of other biochemical indicators suggested that subchronic Cd2+ exposure possibly triggered the onset of AD through the intervention of lipid peroxidation pathway. Furthermore, in vivo monitoring the downtrend of Aβ42% in cerebrospinal fluid (CSF) could also be realized, which offers a great opportunity for early diagnosis and treatment of AD that may be induced by environmental factors with CSF Aβ42% as a reliable indicator.
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JOURNAL OF MOLECULAR STRUCTURE
·
2024
·
IF 4
Hu Wang,Pengxiao Guo,Yadong Zhou,Chaochuang Yin,Yizhu Lei,Renshu Wang,Yinyan Wang,Tingting Wu,Ziao Zong
Two mononuclear Copper(II) complexes, identified as [Cu(C 10 H 8 NO 4 F)(C 6 H 7 N)] ( C1 ) and [Cu(C 10 H 8 NO 4 F)(C 12 H 8 N 2 )]·H 2 O·CH 3 OH ( C2 ), incorporating a tridentate Schiff-base ligand with an ONO coordination (C 10 H 8 NO 4 F = 5-fluoro-2-hydroxybenzylidene-L‑serine) and two unique auxiliary ligands (C 6 H 7 N = 4-methylpyridine and C 12 H 8 N 2 = 1,10-phenanthroline) were developed and detailed structurally. Density functional theory (DFT) evaluations of these complexes employed Becke's three-parameter hybrid (B3LYP) approach within the Gaussian 16 computational package. The outcomes from computational analysis corresponded with experimental data. Additionally, the inhibition capabilities of complexes C1 and C2 were evaluated in vitro targeting jack bean urease. Simultaneously, molecular docking was utilized to determine potential binding interactions. Experimental results and docking analyses showed that C1 had considerable inhibitory strength (IC 50 = 2.44 ± 0.15 μM) relative to the benchmark control, acetohydroxamic acid (IC 50 = 27.73 ± 2.93 μM). Furthermore, a 100-ns molecular dynamics assessment was performed to examine the interaction stability of urease with C1 and C2 , using the Desmond 2021 tool from Schrödinger. The correlation between structural configurations and inhibition efficacy was further explored through molecular docking, density functional theory analysis, and molecular dynamics evaluations.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zhilei Guo,Guohua Jing,Sara A. Tolba,Chung-shin Yuan,Yu-Hua Li,Xiaowei Zhang,Zhiwei Huang,Huawang Zhao,Xiaomin Wu,Huazhen Shen,Wenjie Xia
Transition metal oxide (TMO)-decorated TiO 2 catalysts excel at low-temperature Hg 0 oxidation. However, TMOs are typically found in large nanoparticles (NPs), resulting in a lower atom utilization efficiency. The current paper presents the design of an Au single atom (SA)-doped Ti 4+ defected TiO 2 (Au SAC-Ti 1-x O 2 ) and investigations concerning the influence of an O-Au-O coordination environment on Hg 0 oxidation. Au SAC-Ti 1-x O 2 was designed using an O-Au-O coordination environment and the O-Au-O orbital interaction was elucidated using density functional theory (DFT). The enhanced oxidative capability of lattice oxygen atoms and the interaction between Hg 0 and oxygen atoms were investigated. The O-Au-O coordination environment containing Au SAC Ti 1-x O 2 was then synthesized and characterized using X-ray absorption fine structure (XAFS), X-ray photoelectron spectroscopy (XPS), etc. Finally, Hg 0 oxidation catalytic activity was determined. Due to the increasing population of Au-O antibonding orbital interactions in the valence band, the bond order of O-Au-O in Au SAC Ti 1-x O 2 decreased significantly, thereby enhancing the oxidation ability of its adjacent oxygen atoms. Au SA and ultra-small Au clusters coexisted on a Ti 1-x O 2 catalyst, and the Hg 0 -oxidation efficiency at 150–200 °C was 14 times and 1.5 times greater than those of TiO 2 and 0.1 % Au/TiO 2 , respectively. Furthermore, Au SAC Ti 1-x O 2 was more resistant to the inhibition of SO 2 and NO. It provides an efficient method for developing highly active SA catalysts for Hg 0 oxidation.
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