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ACS Sustainable Chemistry & Engineering · 2019 · IF 6.97

Ultrasound-Assisted Nitrogen and Boron Codoping of Graphene Oxide for Efficient Oxygen Reduction Reaction

Mingli Zhang,Hengcong Tao,Yongchao Liu,Chao Yan,Song Hong,Justus Masa,Alex W. Robertson,Shizhen Liu,Jieshan Qiu,Zhenyu Sun

Development of naturally abundant, low cost, and energy-efficient electrocatalysts for the oxygen reduction reaction (ORR) is essential for commercialization of fuel cells. In this work, we report simple ultrasonication assisted synthesis of nitrogen and boron dual-doped graphene oxide (NB/GO) and demonstrate its application as an effective ORR catalyst realizing predominantly 4e– reduction of O2 to OH– in 0.1 M KOH. Enhanced ORR electrocatalysis of the dual B and N codoped GO as opposed to GO singly doped with B or N arises from the synergistic interaction of the boron and nitrogen species. The content and configuration of both N and B dopants can be readily tailored by controlling the ultrasonic conditions, thereby permitting tuning of the ORR activity. Furthermore, the developed NB/GO metal-free catalyst exhibited very promising long-term durability and resistance to methanol poisoning compared to the state-of the art Pt/C catalyst.

CAS / MDL: 10043-35-3 34819-78-8
研究领域: 材料科学 · 电化学 · 能源技术
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APPLIED SURFACE SCIENCE · 2017 · IF 3.387

Effect of selenization parameters on hydrogen evolution reaction activity of WSe2 electrodes

Hongchao Li,Jianpeng Zou,Senlin Xie,Xian Leng,Di Gao,Xu Mao

WSe 2 films were prepared on inexpensive graphite substrate through direct-current magnetron sputtering and rapid selenization for catalytic application in the hydrogen evolution reaction (HER). The effects of the temperature and time in selenization process on the HER activity were studied in details. Scanning electron microscopy and Raman spectroscopy indicates that the graphite surface is covered by WSe 2 nanosheets . The HER activity of WSe 2 samples prepared at different conditions has been evaluated via linear sweep voltammetry. Through adjusting selenization parameters, the WSe 2 nanofilms consists of the proper nanosheets has been prepared with the optimal HER activity. It’s important to control the number, the size and crystallinity of WSe 2 nanosheets which take responsibility for the HER activity. WSe 2 electrodes prepared at 500   °C for 10   min exhibit high stability in acidic solution and get the optimal activity with an over potential around −179   mV vs reversible hydrogen electrode (RHE) at the current density of 10   mA   cm −2 .

研究领域: 材料科学 · 电化学 · 纳米材料 · 催化化学 · 能源材料
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Small · 2019 ·Vol. 15 ·期 12 ·1805474 · IF 10.856

Coupling PtNi Ultrathin Nanowires with MXenes for Boosting Electrocatalytic Hydrogen Evolution in Both Acidic and Alkaline Solutions

Yi Jiang,Xingqiao Wu,Yucong Yan,Sai Luo,Xiao Li,Jingbo Huang,Hui Zhang,Deren Yang

Developing an efficient electrocatalyst for the hydrogen evolution reaction (HER) working in both acidic and alkaline solutions is highly desirable, but still remains challenging. Here, Pt x Ni ultrathin nanowires (NWs) with tunable compositions ( x = 1.42, 3.21, 5.67) are in situ grown on MXenes (Ti 3 C 2 nanosheets), serving as electrocatalysts toward HER. Such Pt x Ni@Ti 3 C 2 electrocatalysts exhibit excellent HER performance in both acidic and alkaline solutions, with the Pt 3.21 Ni@Ti 3 C 2 being the best one. Specifically, Pt 3.21 Ni@Ti 3 C 2 achieves record-breaking performance in terms of lowest overpotential (18.55 mV) and smallest Tafel slope (13.37 mV dec −1 ) for HER in acidic media to date. Theory calculations and X-ray photoelectron spectroscopy analyses demonstrate that the coupling of MXenes with the NWs not only approaches the Gibbs free energy for hydrogen adsorption close to zero through the electron transfer between them in acidic media, but also provides additional active sites for water dissociation in alkaline solution, both of them being beneficial to the HER performance.

研究领域: 材料科学 · 电化学 · 纳米催化 · 能源材料 · 物理化学
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ELECTROCHIMICA ACTA · 2016 · IF 4.803

Electrochemical fabrication of porous Ni-Cu alloy nanosheets with high catalytic activity for hydrogen evolution

M.Y. Gao,C. Yang,Q.B. Zhang,Y.W. Yu,Y.X. Hua,Y. Li,P. Dong

Porous Ni-Cu alloy films composed of nanosheets are directly fabricated on Cu substrate using a facile potentiostatic electrodeposition approach from a 1:2 choline chloride-ethylene glycol eutectic solvent (ethaline) containing nickel chloride and copper chloride. Electrochemical co-deposition of Ni-Cu alloy in ethaline is found to be thermodynamically favorable in comparison to conventional aqueous solutions. The deposition process occurs via an instantaneous nucleation and growth of nanoparticles at the initial stage and develops vertically to form nanoporous structures arrayed with nanosheets over deposition time . The as-prepared porous Ni-Cu alloy nanosheet arrays exhibit enhanced electrocatalytic activity for the hydrogen evolution reaction (HER) in alkaline media , which displays a small Tafel slope of 57.2   mV   dec −1 with a low onset potential of −48   mV vs. RHE at an optimal condition. It requires small overpotentials of −128 and −150   mV to drive catalytic current densities of 10 and 20   mA   cm −2 , respectively. This facile electrodeposition method performed in ethaline provides an efficient way to fabricate porous Ni-based alloy nanosheets directly on a current collector, which is a promising technology for the synthesis of earth-abundant HER electrocatalysts .

研究领域: 电催化 · 材料科学 · 能源化学 · 纳米材料 · 电化学
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CHINESE JOURNAL OF CATALYSIS · 2015 ·Vol. 36 ·期 2 ·204-208 · IF 1.964

Simple primary amine catalyzed aerobic reductive ring-cleavage of isoxazole motif

Zhongkui Zhao,Renzhi Li,Yu Li,Guiru Wang

A clean and highly efficient catalytic aerobic reductive ring-cleavage of 3–methylanthra[1,2- c ]isoxazole-6,11-dione to 1-amino-2-acetylanthraquinone was performed using simple organic amines as organocatalysts and water as a green reaction medium. This method provides a new clean transformation of isoxazole-containing compounds to the corresponding ortho -amino ketones . The catalytic performance of various organic amines was carefully screened, and simple organic primary amines were found to be promising practical catalysts with outstanding catalytic performance. Isopropylamine as the organocatalyst gave 97.2% conversion of 3–methylanthra[1,2- c ]isoxazole-6,11-dione, with 97.2% selectivity to 1-amino-2–acetylanthraquinone, in the presence of oxygen only, using 1 equiv. of hydrazine hydrate at room temperature for 3 h. A possible mechanism is also proposed.

研究领域: 有机化学 · 催化化学 · 绿色化学 · 药物化学 · 合成方法学
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Ultrafast kinetics net electrode assembled via MoSe2/MXene heterojunction for high-performance sodium-ion batteries

Enze Xu,Yan Zhang,Hui Wang,Zhifeng Zhu,Junjie Quan,Yajing Chang,Pengcheng Li,Dabin Yu,Yang Jiang

Establishing advanced sodium-ion batteries (SIBs) with high energy density and eco-friendly electrode materials are still far from satisfactory due to the large-size of sodium-ions and sluggish redox kinetics during electrochemical processes. Herein, a novel ultrafast kinetics net electrode assembled via MoSe 2 /MXene heterojunction is synthesized by a simple hydrothermal method followed by thermal annealing. Featuring the Van der Waals force interaction between MoSe 2 and MXene , the volumetric change during the sodium ions insertion/extraction courses is effectively restrained, and the reaction kinetics is greatly enhanced further. Meanwhile, both the high electrical and ion conductivity (lower diffusion barrier between Na + /MXene ~0.066 eV) provided by the unique MXene based net heterostructure of our hybrid materials, as evidenced by DFT calculations, are beneficial to the transportation of sodium ions, thus enabling an outstanding rate and long-cycling capability. As a result, the fabricated cells exhibit high reversible capacities of 490 mAh g −1 at 1 A g −1 , as well as 250 mAh g −1 at a high current of 10 A g −1 with a coulombic efficiency of 99.8%, indicating the excellent electrochemical performance of our hybrid materials, especially at high current. This novel net MoSe 2 /MXene heterostructure, combined with our simple synthesis strategy together, are expected to have great potential in sodium-ions storage application.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米材料 · 固态物理
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CELLULOSE · 2019 ·Vol. 26 ·期 3 ·1961-1976 · IF 3.917

Effective and simple one-step strategy for preparation of “clickable” cellulose modules: support to build antibacterial materials

Sun Lijian,Ding Chunyue,Qian Xueren,An Xianhui

Abstract An efficient and simple way to generate “clickable” cellulose modules called alkyne-functionalized cellulose fibers (ACFs) for click reaction was presented. This method is only based on one step reaction: propargyl methacrylate (PMA) with pendant alkynyl groups was grafted onto the surface of cellulose fibers (CFs) using ceric ammonium nitrate as the initiator in aqueous medium. This has been providing a new and versatile platform for the wide utilization of cellulose resources and creation of novel functional materials. The effect of process variables on grafting copolymerization of PMA was investigated and suitable preparation conditions were identified. The clickability of ACFs was evaluated by reacting with two azides. The antibacterial cellulose functional material was achieved through incorporation of a “clickable” handle (alkynyl groups) to cellulose fibers followed by rapid attachment of β-cyclodextrin with an azide tag using copper-catalyzed click reaction and loading with ciprofloxacin hydrochloride (CipHCl). Pure CFs and ACFs showed a little affinity to CipHCl, whereas click products (ACFs@Azide-β-CD) increased the loading amount dramatically because the equilibrium amount was higher than pure CFs and ACFs. Meanwhile, the release process of CipHCl from ACFs@Azide-β-CD was prolonged to reaches the equilibrium. The ACFs@Azide-β-CD loaded with CipHCl showed excellent antibacterial activity against Escherichia coli . The ACFs@Azide-β-CD loading CipHCl have considerably longer bacterial activity against E. coli compared to CFs and ACFs. Graphical abstract

研究领域: 材料科学 · 生物医学工程
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MATERIALS LETTERS · 2014 · IF 2.269

Colloidal synthesis of chalcostibite copper antimony sulfide nanocrystals

Yu Zou,Jiang Jiang

We report the colloidal synthesis of monodisperse phase pure chalcostibite CuSbS 2 nanocrystals in high boiling point solvent. The use of dodecanethiol as ligands had an advantage over oleylamine on avoiding the hydrolysis of Sb precursor. The effect of reaction temperature and Cu/Sb feed molar ratio on the synthesis of copper antimony sulfide nanocrystals in dodecanethiol system was investigated. As a result of the reactivity difference between Cu and Sb precursors, the formation of CuSbS 2 nanocrystals involves the preferential nucleation of Cu-rich nanocrystals and their subsequent reaction with remaining Sb precursors. The band gap of the resulting CuSbS 2 nanocrystals was measured to be ~1.59   eV.

研究领域: 材料化学 · 纳米科学 · 无机化学 · 半导体材料 · 胶体化学
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Energy Technology · 2019 ·Vol. 7 ·期 9 ·1900374 · IF 3.163

Effect of Supports on the Redox Performance of NiFe2O4 in a Chemical Looping Process

Zhong Ma,Dewang Zeng,Shuai Zhang,Rui Xiao

NiFe 2 O 4 oxygen carrier (OC) presents higher oxygen carrying capacity than single metal oxides (NiO and Fe 2 O 3 ). However, the redox ability of NiFe 2 O 4 gets deactivated due to phase segregation. Herein, the investigation of the effect of supports (CeO 2 , CeZrO 2 , and ZrO 2 ) on the phase stability and the redox performance of NiFe 2 O 4 during the chemical looping (CL) process are presented. The structure of NiFe 2 O 4 -based OCs is characterized using different characterization methods. The CL reaction is conducted in a fixed-bed reactor at 900 °C under alternate 5% CO/N 2 and 5% O 2 /N 2 atmospheres. The results indicate that the redox performance and the phase stability of NiFe 2 O 4 -based OCs are significantly affected by the supports. According to experimental results, CeO 2 can improve the oxygen mobility of NiFe 2 O 4 . The CeO 2 –NiFe 2 O 4 OC has the best performance in terms of both recyclability and phase stability during the redox cycles. The results show that CeO 2 –NiFe 2 O 4 can reduce the tendency of Fe segregation due to the high concentration of oxygen vacancies. It can be reduced and reoxidized to the original crystalline phase of NiFe 2 O 4 . Nevertheless, the CeZrO 2 –NiFe 2 O 4 and ZrO 2 –NiFe 2 O 4 OCs have drawbacks related to serious sintering and phase segregation into Fe 2 O 3 .

研究领域: 材料科学 · 化学工程 · 能源化学 · 催化化学 · 无机化学
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CONSTRUCTION AND BUILDING MATERIALS · 2024 · IF 7.4

Mechanism of interaction between hydration–carbonation of C2S

Kai Luo,Wensheng Zhang,Jiayuan Ye,Jun Li,Zhongyuan Lu,Xuehong Ren

The physical and microscopic properties of γ-C 2 S and β-C 2 S under hydration, carbonation , and hydration–carbonation cycle reactions were investigated. The hydration–carbonation cycle reaction facilitated the carbon sequestration of C 2 S, and the generation of CaCO 3 filled the pores of the matrix and enhanced the matrix density in the carbon fixation reaction process. In the subsequent hydration and reaction process, the formation of hydration products increased the number of pores in the matrix and reduced the matrix density. Post-hydration, γ-C 2 S slurry became powder and had no mechanical strength . However, after carbonation reaction and two carbonation–hydration cycles, γ-C 2 S exhibited better mechanical properties than β-C 2 S.

研究领域: 材料科学 · 硅酸盐化学 · 建筑材料 · 碳捕集与封存 · 无机非金属材料
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Journal of Materials Research and Technology-JMR&T · 2022 · IF 6.267

Enhanced negative thermal expansion property in (KMg)xSc2-x(WO4)3 ceramics synthesized by solid–state reaction

Zhiping Zhang,Yuenan Wang,Yang Lei,Fang Zhang,Xiaobing Chen,Hongfei Liu

Negative thermally expanded (NTE) (KMg) x Sc 2-x (WO 4 ) 3 (0 = x ≤ 1.5) ceramics have been prepared via solid-state reaction. X-ray diffraction (XRD) analysis reveals that (KMg) x Sc 2-x (WO 4 ) 3 undergoes a composition-induced phase transition as the (KMg) 3+ -substitution content increases. For x = 0.25, both hexagonal (KMg) x Sc 2-x (WO 4 ) 3 and orthorhombic Sc 2 (WO 4 ) 3 coexisted in the sample. For 0.25 < x ≤ 1, a single-phase, hexagonal (KMg) x Sc 2-x (WO 4 ) 3 , was obtained. When x is further increased to 1.25, monoclinic MgWO 4 impurity was detected in the sample. Meanwhile, as x increases, the grain size of (KMg) x Sc 2-x (WO 4 ) 3 ceramics grows up. Hexagonal (KMg) x Sc 2-x (WO 4 ) 3 ceramics show high densification and strong NTE property. Thermomechanical analysis indicates that the linear coefficients of thermal expansion (CTEs) of hexagonal (KMg) x Sc 2-x (WO 4 ) 3 ceramics decrease from −7.48 × 10 −6  °C −1 to −14.06 × 10 −6  °C −1 with the increase of x. High-temperature XRD analysis reveals that hexagonal (KMg) 0.5 Sc 1.5 (WO 4 ) 3 show an anisotropic NTE. The intrinsic linear CTEs are α a  = α b  = −6.74 × 10 −6  °C −1 , α c  = 11.03 × 10 −6  °C −1 and the volumetric CTE is α v  = −2.52 × 10 −6  °C −1 .

研究领域: 材料科学 · 无机非金属材料 · 功能陶瓷 · 热学性能 · 结构与物性
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ELECTROCHIMICA ACTA · 2022 · IF 7.336

Deep eutectic solvents regulation synthesis of multi-metal oxalate for electrocatalytic oxygen evolution reaction and supercapacitor applications

Hongying Yang,Zhenfeng Cheng,Pengchao Wu,Yahui Wei,Jingyun Jiang,Qun Xu

Design and fabrication of 2D multi-metal oxalate materials with desired electrochemical activities are highly needed in electrocatalysis and supercapacitors . Herein, assisted by the deep eutectic solvothermal (DES) method, multi-metal oxalate consisting of Fe, Co, Ni, Cu, and Zn with different morphology was the controlled synthesis. It was found that the structure and composition of DES can control the nucleation and growth of multi-metal oxalate. High molecular PEG and gradually slow-release oxalic acid are in favor of the formation of 2D structure, while the low molecular EG and abundant oxalic acid are positive for the formation of 3D nanoparticles. The properties of the obtained multi-metal oxalates are confirmed by multi-analysis, which involves the single Ni-oxalate phase, morphological evolution ranging from particles to nanosheets, and complex composition up to five metal elements including Fe, Co, Ni, Cu as well as Zn. Notably, the well-designed 2D (FeCoNiCuZn)(C 2 O 4 )·2H 2 O nanosheets exhibit an ultralow overpotential of 334 mV at 100 mA cm −2 for OER as electrocatalyst with prolonged durability over 30 h at 10 mA cm −2 and a high specific capacity of 1337 C g −1 for aqueous supercapacitor.

研究领域: 材料化学 · 电化学 · 纳米材料 · 能源存储 · 催化化学
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