Small
·
2022
·Vol. 19
·期 8
·2206071
·
IF 15.153
Fangqing Wang,Ying Li,Rui Zhang,Hui Liu,Yangyang Zhang,Xuerong Zheng,Jun Zhang,Cong Chen,Shijian Zheng,Huolin L. Xin
Atomically dispersed nitrogen-coordinated 3d transition-metal site on carbon support (M-NC) are promising alternatives to Pt group metal-based catalysts toward oxygen reduction reaction (ORR). However, despite the excellent activities of most of M-NC catalysts, such as Fe-NC, Co-NC et al., their durability is far from satisfactory due to Fenton reaction. Herein, this work reports a novel Si-doped Ni-NC catalyst (Ni-SiNC) that possesses high activity and excellent stability. X-ray absorption fine structure and aberration-corrected transmission electron microscopy uncover that the single-atom Ni site is coordinated with one Si atom and three N atoms, constructing Ni-Si 1 N 3 moiety. The Ni-SiNC catalyst exhibits a half-wave potential (E 1/2 ) of 0.866 V versus RHE, with a distinguished long-term durability in alkaline media of only 10 mV negative shift in E 1/2 after 35 000 cycles, which is also validated in Zn-air battery. Density functional theory calculations reveal that the Ni-Si 1 N 3 moiety facilitates ORR kinetics through optimizing the adsorption of intermediates.
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ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Yudi Wang,Jialong Duan,Yuanyuan Zhao,Xiya Yang,Qunwei Tang
Developing efficient and cost-effective counter electrodes (CEs) to catalyze triiodide reduction reaction is a persistent objective for high-performance dye-sensitized solar cells (DSSCs). One promising solution is to design electron-enriched electrode materials by combining conductive polymers with alloys. In this work, ternary hybrid PtM@polyaniline (M = Ni, FeNi) CEs are synthesized by one-step replacement reaction and in-situ polymerization reaction. When assembling into liquid-junction DSSCs, the power conversion efficiencies of 8.52% and 8.39% for the devices tailored with PtNi@polyaniline and PtFeNi@polyaniline CEs can be obtained. The experimental results demonstrate that the enhanced photovoltaic performances are mainly attributed to matching work function and high electrocatalytic activity of these well-designed hybrid CEs. Arising from the competitive reactions between transition metal and I 2 /I 3 − species, the dissolution reaction of Pt in liquid electrolyte is restricted and therefore the long-term stability of corresponding devices are significantly enhanced.
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ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Wenli Pei,Xiaoyang Wang,Chunhong Liu,Dong Zhao,Chun Wu,Kai Wang,Qiang Wang
Hyperbranched transition metal phosphides (TMPs) nanocrystals are an interesting class of materials, which can be used as an efficient catalyst for hydrogen evolution reaction (HER). However, big challenge remains for the preparation of ternary hyperbranched TMPs, and relationship between their HER performances and the splitting degree is also not well understood. Here, hyperbranched Co-Ni-P nanocrystals with different splitting degrees were prepared via a novel strategy, and their alkaline HER performances were studied. During the synthesis process, hyperbranched Co 2 P nanocrystals were used as template, and Ni precursors were injected into the reaction solution at different holding stage. When the Ni precursor was injected earlier, the podgy particles with low splitting degree would be obtained. Conversely, delaying the injection of Ni precursor would lead to high splitting degree. The formation process of ternary phase was also studied. After Ni precursor was injected, a Co-Ni-P amorphous layer was formed on the surface of the Co 2 P particles, and then the Ni atoms diffused into the Co 2 P phase to form Co-Ni-P nanocrystals. Electrochemical performances tests show that the splitting degree has great impact on HER performances. The higher splitting degree usually leads to larger electrochemical surface area, and higher catalytic activity can be achieved. The sheaf-like Co-Ni-P nanocrystals demonstrate a small overpotential of 119 mV at current density of 10 mA cm −2 , and good durability over 23 h in 1 M KOH solution. We believe that this work can help understand the relationship between the HER performances of hyperbranched TMPs nanocrystals and their splitting degree, and provide a synthetic strategy for the preparation of highly efficient TMPs catalysts.
研究领域:
材料科学
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电化学
·
纳米技术
·
催化
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LANGMUIR
·
2011
·
IF 4.269
Changdong Gu,Jiangping Tu
We report a procedure to fabricate nanostructured Ni films via programmed electrochemical deposition from a choline-chloride-based ionic liquid at a high temperature of 90 °C. Three electrodeposition modes using constant voltage, pulse voltage, and reverse pulse voltage produce a variety of nanostructured Ni films with micro/nanobinary surface architectures, such as nanosheets, aligned nanostrips, and hierarchical flowers. The nanostructured Ni films possess face-centered cubic crystal structure. Amazingly, it is found that the electrodeposited Ni films deliver the superhydrophobic surfaces without any further modifications by low surface-energy materials, which might be attributed to the vigorous micro/nanobinary architectures and the surface chemical composition. The electrochemical measurements reveal that the superhydrophobic Ni film exhibit an obvious passivation phenomenon, which could provide enhanced corrosion resistance for the substrate in the aqueous solutions.
研究领域:
材料科学
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电化学
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纳米技术
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表面工程
·
腐蚀科学
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INORGANIC CHEMISTRY
·
2019
·
IF 4.85
Changwei Chen,Xiangbo Feng,Qing Zhu,Rui Dong,Rui Yang,Yan Cheng,Chi He
In the present work, a series of MOF-74 (Ni) materials with narrow micropore channels and abundant unsaturated metal sites was respectively prepared via hydrothermal (HT), condensation reflux (CE), and microwave-assisted (MW) methods. The physicochemical properties of synthesized materials were characterized by powder X-ray diffraction, N2-sorption, field-emission scanning electron microscopy, Fourier-transform infrared (FTIR), thermogravimetric (TG)/TG-FTIR, X-ray photoelectron spectroscopy, UV–vis–near infrared, NH3/CO2-temperature programmed desorption, and in situ diffuse reflectance infrared Fourier transform spectroscopy. Their CO2/N2 adsorption performances were evaluated by isotherm adsorption and dynamic adsorption experiments. We found that the MW is a rapid and facile protocol for the synthesis of MOF-74 (Ni) materials with highly efficient CO2 capture capacity. The well-shaped MW-140 adsorbent with superior CO2 adsorption capacity of 5.22 mmol/g at 25 °C can be obtained within 60 min by the MW process, almost 6 times higher than that of the commercial activated carbon (0.89 mmol/g). Results of dynamic adsorption experiments showed that the MW-140 material possesses the highest CO2 adsorption capacity of 3.37 mmol/g under humid conditions (RH = 90%). Importantly, MW-140 has excellent adsorption stability and recyclability, superior CO2 capture selectivity (CO2/N2 = 31), and appropriate isosteric heat in CO2 adsorption (21–38 kJ/mol), making it a promising and potential material for industrial CO2 capture. Characterization results demonstrated that the high capture capability of MOF-74 (Ni) materials can be attributed to the synergistic effect of abundant narrow micropore channels and rich five-coordinated Ni2+ open metal sites which are beneficial for the trapping of CO2 molecules.
研究领域:
材料科学
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环境化学
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无机化学
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碳捕集与封存
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纳米材料
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2022
·
IF 3.428
Yan Fu,Ye Li,Jun Zhang,Dongxue Liu,Chang Liu,Yi Ke
Antimony is a new type of pollutant with potential toxicity and carcinogenicity. Therefore, the restoration of antimony-contaminated water has attracted wide attention from all over the world. In this research, we synthesized chloride intercalated Ni-Al layered double hydroxide (Ni-Al LDH) with a good laminated structure by co-precipitation and ion exchange. We investigated the adsorption performance of Ni-Al LDH for Sb(V) in a one-component system for the first time through a series of batch experiments. The effect of key process variables, such as pH, reaction temperature, adsorbent dosage, contact time and initial concentration on the adsorption was studied in single-factor experiments separately. The reaction rapidly reached adsorption equilibrium within 30 min and it maintained the antimony removal rate at about 91% at the optimum reaction conditions. Multiple models were applied to fit the adsorption isotherm, kinetic and thermodynamic data to describe the adsorption behaviors of Sb(V) on Ni-Al LDH. A perfect fit between the Langmuir model and isothermal adsorption experimental data confirmed a maximum adsorption capacity of material could be up to 142.86 mg/g. SEM-EDS, XPS, and other characterization analyses demonstrated that ion exchange and ligand exchange are the primary mechanisms for triggering the adsorption process. It proved the excellent regeneration performance of the material by data from five stable adsorption/desorption cycles. It could be demonstrated that Ni-Al LDH could be an applicable adsorbent for the removal of Sb(V) .
研究领域:
环境科学
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材料化学
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水处理
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吸附技术
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污染物去除
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JOURNAL OF POROUS MATERIALS
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2026
·
IF 3.2
Guo Hanxu,Fu Sen,Yuan Hong
Hierarchical zeolites can provide multidimensional spatial networks, thereby holding significant potential as catalysts for BTX production from biomass pyrolysis. In this study, nano-ZSM-5 zeolite (Z X-X ) with a hierarchical pore structure was synthesized using glycine as a growth inhibitor. Due to the exceptional ability of Ni to cleave C–C and C–H bonds, Ni modification was performed on the Z 30-0.2 catalyst. The effects of glycine and Ni loading on the morphology and pore structure of the zeolites were systematically investigated using scanning electron microscopy (SEM), transmission electron microscopy (TEM), and N 2 adsorption–desorption. The results demonstrated that the particle size of 10 wt% Ni-Z 30-0.2 zeolite ranged from 200 to 300 nm, with a BET surface area of 314 m 2 /g and abundant mesopores. The NH 3 -TPD results showed that the acid amount of 10 wt% Ni-Z 30-0.2 was 0.72 mmol/g. The prepared zeolite was employed in a fixed-bed reactor to catalyze the pyrolysis of oleic acid for the production of benzene, toluene, and xylene (BTX). The introduction of metal Ni significantly enhanced the BTX yield. At 500 ℃, the average BTX yield achieved with the 10 wt% Ni-Z 30-0.2 catalyst was 19.4 wt%, which was higher than that of the zeolite without Ni loading.
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ENERGY CONVERSION AND MANAGEMENT
·
2026
·
IF 10.9
Shiying Yang,Fan Jiao,Xiaotong Fan,Lixinyu Mei,Xiaojing Shi,Qibin Liu
Methane carbon cyclic reforming (MCCR) represents a novel dry methane reforming (DMR) reaction, offering advantages in terms of greenhouse gas utilization and automatic product separation. This study dedicated to exploring the potential of the MCCR method for continuous and long-term production of H 2 and CO fuels. Using a self-synthesized Ni/Al 2 O 3 catalyst, we elucidated at the microscopic level the advantages of directional conversion of carbon and hydrogen elements during the MCCR process, as well as its underlying mechanism. Through in-situ testing and microscopic characterization, it was confirmed that the decoupling of the MCCR reaction can suppress side reactions, and prevent excessive graphitization of carbon deposits and promote their removal by switching reaction mechanisms promptly. The long-term continuous fuel production experiment was conducted at the macroscopic level for validating these findings. The catalyst’s stability was confirmed by 2750 min of continuous TGA cycling tests, maintaining a carbon removal ratio of 99.99% after 250 cycles. This performance was further validated in a fixed-bed reactor, where an average H-C ratio of 1.13 was sustained over 40 cycles during a 20-hour long-term test. This research paves the way for the advancement of MCCR technology and complements conventional DMR methods for the production of clean fuel.
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Science China-Chemistry
·
2026
·
IF 9.7
Xiong Yang-Yang,Dai Qing-Hua,Deng Songlin,Wei Zhang-Wen,Liang Zi-Ying,Chen Yin-Xian,Geng Wei,Chen Cheng-Xia,Su Cheng-Yong
Constructing the dual-catalytic scaffolds with the pinpointed photoredox/organometallic sites is pivotal for metallaphotocatalysis, yet challenging. Herein, we demonstrate a versatile protocol of sequential dynamic assembly (SDA) for precise and quantitative installation of Ir-photoredox and Ni-cross-coupling catalysts into a robust metal-organic framework (MOF) to construct an Ir/Ni-catalyst LIFM-XYY-12. Remarkably, LIFM-XYY-12 presents excellent catalytic activity in photoredox-mediated Ni-catalysing cross-coupling reactions between various amines/thiols and aryl halides with yields up to 99%, especially for C–N coupling reaction, achieving fast catalytic reaction kinetics, which is nearly 20-fold than that of the homogeneous system, attributable to the installation of Ir III - and Ni II -sites in close proximity to effectively accelerate electron transfers from Ir- to Ni-centers. Moreover, high S -arylation chemoselectivity (⩾91%) is achieved for various aminothiols carrying primary and secondary arylamine groups, affording a variety of aminothioethers without resorting to protecting group chemistry. The underlying reaction mechanism has been detangled through comprehensive experiments and theoretical calculations. This work highlights SDA as a promising strategy to merge photoredox and transition-metal catalysis into MOF platform for a broad utility in organic transformations.
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Science China-Chemistry
·
2026
·
IF 9.7
Lv Enmin,Diao Jiefeng,Wang Yilong,Yu Hongtao,Henkelman Graeme,Zhang Hao,Zhang Xuefeng,Dong Xinglong
Developing efficient non-precious oxygen reduction reaction (ORR) catalysts remains a critical challenge. Herein, a direct current (DC) arc plasma strategy was demonstrated to construct nitrogen-doped carbon-coated Ni-ZrC heterostructured nanoparticles ((Ni/ZrC)@NC NPs) with precisely tuned interfacial built-in electric fields (BIEFs). Theoretical studies reveal that the significant work function difference (Δ Φ ) drives an asymmetric charge redistribution at the Ni-ZrC heterointerface, shifting d-band centers to optimize the adsorption energy of oxygen intermediates and to reduce reaction energy barriers. In situ optical emission spectroscopy (OES) captures the dynamic plasma evolution (electron temperature ( T e ) at local thermal equilibrium (LTE): 10,330.9 K), elucidating real-time atomic/ionic flux variations and formation mechanism of the core-shell structure and heterostructure. The synergistic Ni-ZrC core and N-doped carbon shell cooperatively enhance charge transfer kinetics and expose abundant active sites. The resulting catalyst achieves exceptional ORR activity with a half-wave potential ( E 1/2 ) of 0.82 V, surpassing Pt/C (0.80 V), alongside superior methanol tolerance and 4e − selectivity. When deployed in both liquid and all-solid-state flexible zinc-air batteries (FZABs), the catalyst delivers superior metrics: peak power densities of 251.63 mW cm −2 (liquid) and 184.22 mW cm −2 (flexible), and stable operation for a long time. This work establishes a paradigm for manipulating interfacial electronic structures via BIEFs engineering, providing a versatile platform for high-performance energy conversion technologies.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2025
·Vol. 36
·期 30
·1912
·
IF 2.8
Wen Jiawei,Zhang Songyang,Chen Jian-an,Zhang Xiaoming,Wang Xin,Huang Guoyong
Titanium niobium oxide (TiNb 2 O 7 , TNO) has become a high-performance anode material for fast-charging lithium-ion batteries due to its high specific capacity, safety advantages and stable cycling performance. Nevertheless, the material’s low electronic/ionic conductivity remains a critical challenge for commercial implementation. The present study presents a novel Ni-doping strategy for TNO that optimizes the electronic structure, achieving a remarkable improvement in lithium-ion storage performance through enhanced charge transfer and ionic diffusion. The Ni 0.02 -TNO anode exhibits a reversible capacity of 240.7 mAh g −1 after 150 cycles at 1C, while retaining 172.9 mAh g −1 even after 1000 cycles under an ultra-high rate of 10C, demonstrating exceptional long-term stability and rate capability. Furthermore, the assembled LiFePO 4 (LFP) ||Ni 0.02 -TNO pouch cell demonstrates outstanding cycling stability, with 86.9% capacity retention over 500 cycles at 1C. Density functional theory calculations reveal that Ni doping reduces the bandgap from 2.193 eV to 0.765 eV, thereby enhancing electronic conductivity and facilitating faster charge transfer kinetics. This work provides a viable pathway for designing advanced lithium-ion batteries with rapid-charging capability and long-term cyclability.
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CATALYSIS TODAY
·
2018
·
IF 4.667
Dawang Chu,Chen Zhao
The effective and selective conversion of cellulose to valuable fuels and chemicals is highly attractive. In this paper, we prepared a catalyst with the adjacent surface Cu° and oxygen-deficient WO x (2 < x < 3) species by reduction of CuWO 4 precursor, and such catalyst coupled with Ni/activated carbon (AC) attained high yield (71 wt%) and good cycling performances in catalyzing one-step hydrothermal conversion of cellulose to ethylene glycol (EG), highly superior to the performances on physically mixed Ni/C, Cu/C and WO 3 . The increased Cu doping amounts led to a higher ratio of the lower valence state W (V or IV) to the high valence W(VI) as indicated by XPS, XRD, and TPR-H 2 analyses. The oxygen vacancies on the hydrogen-reduced CuWO 4 sample dramatically increased, probably due to the benefits from the substantial dissociated H• on the neighboring Cu° center. The EG yields from cellulose are shown to be proportional to the concentrations of oxygen vacancies on WO x , which catalyzes the important elementary retro-aldol step reaction via adsorbing C 6 sugar intermediates in a specific way. It is inferred that Cu introduction is mainly used to create more oxygen vacancies on the WO x surface that helps adsorbing oxygenates, while Ni fast hydrogenates of hydroxyacetaldehyde to EG and avoids coking, constructing a multi-functional synergistic catalytic process from converting of cellulose to EG in the high-temperature water
研究领域:
催化化学
·
生物质转化
·
绿色化学
·
材料化学
·
能源化学
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