CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Chun Yin,Fulin Yang,Shuli Wang,Ligang Feng
Efficient heterogeneous catalysts play a very important role in the value-updated green hydrogen production from urea-containing wastewater. Herein, NiSe 2 /MoSe 2 heterostructured catalyst with optimized interfacial electron redistribution and urea adsorption energies via a strong built-in electric field was demonstrated effective for the urea-assisted water splitting reactions. Efficient catalytic performance was found on NiSe 2 /MoSe 2 hybrid microsphere owing to the combined merits such as the unique structure features, the strong synergetic coupling effects, the increased active sites, and the high amount of intrinsic Ni 3+ species. Excellent urea oxidation activity was found to drive 10 mA cm −2 at the potential of 1.33 V when loaded on the glassy carbon electrode, and a cell voltage of 1.47 V was required in the NiSe 2 /MoSe 2 ||Pt/C urea-water electrolyzer to drive 10 mA cm −2 , about 220 mV less than that of water electrolysis, indicating a less energy consumption technique during the electrolysis. The spectroscopic and theoretical analysis revealed the effective synergy of the Ni–Se bond and Mo–Se bond that would be promising for efficient catalyst system construction.
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Advanced Science
·
2023
·Vol. 10
·期 30
·2303414
·
IF 15.1
Hu Li,Guo-Qin Yang,Xiao-Yang Hu,Yi-Hua Hu,Rui-Bo Zeng,Jin-Rui Cai,Li-Quan Yao,Li-Mei Lin,Li-Ping Cai,Guilin Chen
Sb 2 S 3 is rapidly developed as light absorber material for solar cells due to its excellent photoelectric properties. However, the use of the organic hole transport layer of Spiro-OMeTAD and gold (Au) in Sb 2 S 3 solar cells imposes serious problems in stability and cost. In this work, low-cost molybdenum (Mo) prepared by magnetron sputtering is demonstrated to serve as a back electrode in superstrate structured Sb 2 S 3 solar cells for the first time. And a multifunctional layer of Se is inserted between Sb 2 S 3 /Mo interface by evaporation, which plays vital roles as: i) soft loading of high-energy Mo particles with the help of cottonlike-Se layer; ii) formation of surficial Sb 2 Se 3 on Sb 2 S 3 layer, and then reducing hole transportation barrier. To further alleviate the roll-over effect, a pre-selenide Mo target and consequentially form a MoSe 2 is skillfully sputtered, which is expected to manipulate the band alignment and render an enhanced holes extraction. Impressively, the device with an optimized Mo electrode achieves an efficiency of 5.1%, which is one of the highest values among non-noble metal electrode based Sb 2 S 3 solar cells. This work sheds light on the potential development of low-cost metal electrodes for superstrate Sb 2 S 3 devices by carefully designing the back contact interface.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 48
·2306668
·
IF 19
Yingqian Cen,Yudi Tu,Jingting Zhu,Yutao Hu,Qiaoyan Hao,Wenjing Zhang
Devices based on 2DMs van der Waals (vdW) heterostructures always compose of multiple contacts. Due to the instability of nanoscale 2DMs and interfaces, these contacts can be affected by the operation-induced photo or thermal effect. They can trigger the evolution of junctions and rearrange the junctions across a device, which are detrimental for applications. Herein, vdW heterostructure of indium selenide (InSe) and black phosphorus (BP) on Au electrodes are investigated to reveal the contact evolution and its relation to device performance. During operation, light irradiation changes the I–V characteristics from symmetry to strong rectification. Photocurrent mapping and Kelvin-probe force microscopy (KPFM) reveal triple junctions in this heterostructure, i.e., Au-InSe junction, InSe homojunction, and InSe-BP heterojunction. The variation of I–V characteristics of vdW heterostructure is ascribed to the evolution of Au-InSe junction from quasi-ohmic junction with a near-zero work function difference ( Δφ ) to a strong Schottky junction ( Δφ = ≈0.27 eV). The stabilized device demonstrates distinguished time-domain response at individual junctions and overall device, indicating the evolution of contacts and the consequent opposite junction directions degrade the overall device performance. This research emphasizes the importance of dealing with heterogeneous contacts and junction directions in designing vdW heterostructure photodetectors.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ziyuan Xiu,Feng Wei,Xin Zhou,Xiaojun Han
Achieving high ammonia yield and Faraday efficiency is a long-sought-after goal in electrochemical N 2 fixation. Yet, the competitive hydrogen evolution in nitrogen reduction process and the low local concentration of nitrogen on the working electrode still limited the electrocatalytic performance. In the present contribution, a Fe-MoSe 2 nanosheet functioned with C18-thiol as a nano-hydrophobic surface was rationally constructed, which efficiently facilitated the three-phase contact of gas (N 2 ), liquid (H 2 O electrolyte), and solid (electrocatalyst). The fabrication of modified hydrophobic surface not only overcame the mass transfer limitation of N 2 and increased the local concentration of N 2 molecules on the catalyst, but also reduced the proton contact with electrocatalyst to inhibit HER. The three-phase electrocatalytic system achieved a high NH 3 yield of 34.75 μg h −1 mg −1 and outstanding Faraday efficiency of 23.31%. The adsorption and activation processes during NRR process were systematically investigated by the combination of experimental results and density function theory (DFT) simulations.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Qiduo Chen,Shan Tang,Dong Feng,Yuhui Xie,Feng Wu,Delong Xie,Yi Mei,Tianbiao Zeng
As a typical conversion alloyed anode material , Germanium selenide (GeSe 2 ) exhibits isotropic lithiation behavior and high theoretical charge-discharge specific capacity. However, pure GeSe 2 anode faces significant volume expansion (∼250 %−360 %) and further exploration is needed in the preparation of flexible electrode materials and structural design. Herein, a simple strategy is designed to load GeSe 2 /C-2 nanoparticles with porous carbon-coated structure on a flexible cross-networking substrate. The 3D network substrate is composed of highly conductive carbon nanotubes and adhesive cotton cellulose fibers. A two-step method involving coating and cross-linking is designed to achieve the fabrication of self-supporting flexible electrodes. As an anode for LIBs , the one layer GeSe 2 discs with ∼0.65 mm thickness manifest capacities of 827.1, 744.4, 676.3, and 472.9 mAh g −1 at 0.1, 0.2, 0.5, and 1 A g −1 , respectively. This superior Li + storage performance can be attributed to the positive collective impact from the integration of nano-scale material, low crystalline properties, and carbon sponge skeleton. Furthermore, the GITT tests indicate that the diffusion coefficient of Li + in the GeSe 2 -based electrodes ranged from 10 −15 to 10 −12 cm 2 /s, and the thickness of the flexible electrode (including two layers) has a negligible impact on its electrochemical performance.
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ACS Nano
·
2023
·
IF 17.1
Chao Li,Yuxing Wu,Qinjun Chen,Yifan Luo,Peixin Liu,Zheng Zhou,Zhenhao Zhao,Tongyu Zhang,Boyu Su,Tao Sun,Chen Jiang
Reperfusion injury presents a significant obstacle to neuronal survival following successful recanalization in ischemic stroke, which is characterized by intricate pathophysiological processes comprising numerous interconnected pathways. Oxidative stress-induced neuronal ferroptosis and the overactivation of glial cells play important roles in this phenomenon. In this study, we developed a targeted cross-linked micelle loaded with idebenone to rescue the ischemic penumbra by inhibiting neuronal ferroptosis and glial overactivation. In rat models, the CREKA peptide-modified micelles accumulate in the damaged brain via binding to microthrombi in the ipsilateral microvessels. Upon reactive oxygen species (ROS) stimulation, diselenide bonds within the micelles are transformed to hydrophilic seleninic acids, enabling synchronized ROS consumption and responsive drug release. The released idebenone scavenges ROS, prevents oxidative stress-induced neuronal ferroptosis, attenuates glial overactivation, and suppresses pro-inflammatory factors secretion, thereby modulating the inflammatory microenvironment. Finally, this micelle significantly reinforces neuronal survival, reduces infarct volume, and improves behavioral function compared to the control groups. This pleiotropic therapeutic micelle provides a proof-of-concept of remodeling the lesion microenvironment by inhibiting neuronal ferroptosis and glial overactivation to treat cerebral ischemia-reperfusion injury.
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BIOSENSORS & BIOELECTRONICS
·
2023
·
IF 12.6
Caixia Sun,Xue Zhang,Hao Huang,Ya Liu,Xianwei Mo,Yufei Feng,Jiahong Wang,Wenhua Zhou,Paul K. Chu,Xue-Feng Yu,Wenxin Liu
Nanozymes with enzyme-like characteristics have drawn wide interest but the catalytic activity and substrate selectivity of nanozymes still need improvement. Herein, Se-vacancy-rich TiSe 2-x @Au nanocomposites are designed and demonstrated as nanozymes. The TiSe 2-x @Au nanocomposites show excellent peroxidase-like activity and the chromogenic substrate p-phenylenediamine (PPD) can be selectively oxidized to compounds that exhibit an absorption peak at 413 nm that differs from that of self-oxidation or generally oxidized species, suggesting high catalytic activity and strong substrate selectivity. Theoretical calculations reveal that the PPD adsorption geometry at Se vacancies with an adsorption energy of −3.00 eV shows a unique spatial configuration and charge distribution , thereby inhibiting the free reaction and promoting both the activity and selectivity in PPD oxidation . The TiSe 2-x @Au colorimetric system exhibits a wide linear range of 0.015 mM–0.6 mM and a low detection limit of 0.0037 mM in the detection of glucose. The blood glucose detection performance for human serum samples is comparable to that of a commercial glucose meter in the hospital (relative standard deviation < 6%). Our findings demonstrate a new strategy for rapid and accurate detection of blood glucose and our results provide insights into the future design of nanozymes.
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CATALYSIS COMMUNICATIONS
·
2023
·
IF 3.7
Zhenbang Xie,Qihang Liu,Haixin Zhao,Hongtai Chen,Guozhi Jia,E. Lei,Chao Wang,Yongzhu Zhou
The low charge separation and transfer of g-C 3 N 4 hinders its industrial application in photocatalytic hydrogen evolution. Here, we design a novel co-catalyst strategy to integrate Ag 2 Se nanoparticles in situ on the surface of g-C 3 N 4 . The optimized photocatalyst, 15% Ag 2 Se/g-C 3 N 4 , demonstrates remarkable photocatalytic efficiency in the hydrogen evolution rate, reaching to 1102.8 μmol·g −1 ·h −1 , 7 times higher than g-C 3 N 4 . To further elucidate the photocatalytic activity of 15% Ag 2 Se/g-C 3 N 4 , we present a possible mechanism based on various characterizations and density functional theory calculations. This research offers potential insights for the future development of silver chalcogenide composites in photocatalysis.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Yongfeng Bu,Hongyu Zhang,Jinzhi Hu,Wenya Jiang,Qin Kang,Shihao Wang,Yuman Li,Shengda Tang,Hongyu Liang
Metallic selenides are considered as a promising class of alternative anodes for sodium ion batteries due to the high capacity conferred by their hybrid sodium storage mechanism. However, the low reversible volume expansion induced by larger size sodium ion storage greatly limits their cycle life, theoretical capacity mining and electrode thickness enhancement. Herein, a germanium selenide/carbon nanofibers (GeSe/CNFs) sodium storage anode is first reported by taking advantage of the encapsulation and dispersion of electrostatic spinning technology, i.e., GeO 2 is first mixed with polyacrylonitrile and electrospun to form a wrapped structure, followed by in situ pre-oxidation, carbonization, and selenization. For the optimized electrode, it delivers a high capacity up to 567 mAh g −1 based on the mass of GeSe (320 mAh g −1 based on GeSe/CNFs), reaching > 80% of its theoretical capacity, with a > 2300 cycles cycling stability at 1.0 A g −1 . In addition, its capacity barely decays after 700 cycles at near commercial electrode thickness (115 µm, the capacity retention > 47–63% even at the ultrahigh thickness of 187–219 µm). This study opens up new possibilities for the development of Se-based sodium storage anode materials with long life, high capacity and ultra-thick electrode that are expected to meet practical needs.
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Small Methods
·
2023
·
IF 12.4
Shanhong Wan,Shanshan Xiao,Mingquan Li,Xin Wang,Khak Ho Lim,Min Hong,Maria Ibáñez,Andreu Cabot,Yu Liu
Developing cost-effective and high-performance thermoelectric (TE) materials to assemble efficient TE devices presents a multitude of challenges and opportunities. Cu 3 SbSe 4 is a promising p -type TE material based on relatively earth abundant elements. However, the challenge lies in its poor electrical conductivity. Herein, an efficient and scalable solution-based approach is developed to synthesize high-quality Cu 3 SbSe 4 nanocrystals doped with Pb at the Sb site. After ligand displacement and annealing treatments, the dried powders are consolidated into dense pellets, and their TE properties are investigated. Pb doping effectively increases the charge carrier concentration, resulting in a significant increase in electrical conductivity, while the Seebeck coefficients remain consistently high. The calculated band structure shows that Pb doping induces band convergence, thereby increasing the effective mass. Furthermore, the large ionic radius of Pb 2+ results in the generation of additional point and plane defects and interphases, dramatically enhancing phonon scattering, which significantly decreases the lattice thermal conductivity at high temperatures. Overall, a maximum figure of merit ( zT max ) ≈ 0.85 at 653 K is obtained in Cu 3 Sb 0.97 Pb 0.03 Se 4 . This represents a 1.6-fold increase compared to the undoped sample and exceeds most doped Cu 3 SbSe 4 -based materials produced by solid-state, demonstrating advantages of versatility and cost-effectiveness using a solution-based technology.
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高影响因子
FUEL
·
2023
·
IF 7.4
Junfeng Qin,Qinghui Shen,Cuicui Du,Min Hong,Yixin Yang,Xiaohua Zhang,Jinhua Chen
Heteroatom doping and vacancy engineering play vital roles in designing a high-activity electrocatalyst . Herein, we proposed a novel enriched Se vacancies engineering of the promising ruthenium chalcogenide of RuSe 2 induced by low-valence Cu doping for promoting hydrogen evolution reaction (HER) electrocatalysis in alkaline media. The Cu-doped RuSe 2 with enriched Se vacancies supported on graphitized carbon (Cu-RuSe 2 @C) was synthesized by a simple one-step selenization of bimetallic MOF precursor of Ru/Cu-BTC (1,3,5-benzenetricarboxylic acid) polyhedra. Compared to the Cu(Ⅱ)-dominant doped RuSe 2 (Cu Ⅱ/Ⅰ -RuSe 2 @C) with deficient Se vacancies, the proposed Cu(Ⅰ)-dominant doped RuSe 2 (Cu Ⅰ/Ⅱ -RuSe 2 @C) with enriched Se vacancies exhibited significantly improved electrocatalytic activity, which was potentially derived from the created electron-deficient Ru δ+ and Se ν− sites induced by low-valence Cu doping. Specifically, Cu Ⅰ/Ⅱ -RuSe 2 @C needed only 40 mV overpotential to drive a HER current density of 10 mA cm −2 , comparable to commercial Pt/C (38 mV) and much lower than those of Cu Ⅱ/Ⅰ -RuSe 2 @C (93 mV) and RuSe 2 @C (362 mV). Furthermore, an alkaline Zn-H 2 O fuel cell with a Cu Ⅰ/Ⅱ -RuSe 2 @C cathode was integrated to demonstrate its potential applications, which delivered a maximum power density of 15.1 mW cm −2 and specific capacitance of 660 mAh g −1 with good stability. Two series-connected alkaline Zn-H 2 O cells acted as a chemical energy converter for simultaneous electricity generation and hydrogen coproduction by driving the coupled water splitting.
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ChemSusChem
·
2021
·Vol. 14
·期 7
·1710-1719
·
IF 8.928
Liwei Shi,Hailiang Fang,Xiaoxia Yang,Jie Xue,Caifeng Li,Shifeng Hou,Cheng Hu
Graphical Doping for batteries : Fe-doped NiSe 2 nanosheets grown on activated carbon cloth substrates provide elevated performance as Li−S free-standing cathodes. Fe-doping in NiSe 2 enables improved charge transfer and stronger interactions with the adsorbed sulfur species, as well as higher electrical conductivity. The transformation of Li 2 S 2 /Li 2 S growth from conventional 2D films to 3D particles eliminates the barriers of phase transitions during the cathode redox processes. The commercialization of Li−S batteries is hindered by the shuttling of lithium polysulfides (LiPSs), the sluggish sulfur redox kinetics as well as the low sulfur utilization during charge/discharge processes. Herein, a free-standing cathode material was developed, based on Fe-doped NiSe 2 nanosheets grown on activated carbon cloth substrates (Fe-NiSe 2 /ACC) for high-performance Li−S batteries. Fe-doping in NiSe 2 plays a key role in the electronic structure modulation of NiSe 2 , enabling improved charge transfer with the adsorbed LiPSs molecules, stronger interactions with the active sulfur species and higher electrical conductivity. Effective promotion of the sulfur redox kinetics and enhanced sulfur utilization were achieved under high areal sulfur loadings. The stronger interactions with LiPSs together with the unique 3D structure of Fe-NiSe 2 /ACC also induced the transformation of Li 2 S 2 /Li 2 S growth from conventional 2D films to 3D particles, significantly eliminating the barriers of solid nucleation and growth during the phase transition of liquid LiPSs to solid Li 2 S 2 /Li 2 S. With a high sulfur loading of 9.9 mg cm −2 , the Fe-NiSe 2 /ACC cathode enabled a high area capacity of 9.14 mAh cm −2 with a low average decay of 0.11 % per cycle over 200 cycles at 0.1 C.
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