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High-entropy catalysts for electrochemical water-electrolysis of hydrogen evolution and oxygen evolution

《能源前沿(英文)》 doi: 10.1007/s11708-023-0892-6

摘要: High entropy materials (HEMs) have developed rapidly in the field of electrocatalytic water-electrolysis for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) due to their unique properties. In particular, HEM catalysts are composed of many elements. Therefore, they have rich active sites and enhanced entropy stability relative to single atoms. In this paper, the preparation strategies and applications of HEM catalysts in electrochemical water-electrolysis are reviewed to explore the stabilization of HEMs and their catalytic mechanisms as well as their application in support green hydrogen production. First, the concept and four characteristics of HEMs are introduced based on entropy and composition. Then, synthetic strategies of HEM catalysts are systematically reviewed in terms of the categories of bottom-up and top-down. The application of HEMs as catalysts for electrochemical water-electrolysis in recent years is emphatically discussed, and the mechanisms of improving the performance of electrocatalysis is expounded by combining theoretical calculation technology and ex-situ/in situ characterization experiments. Finally, the application prospect of HEMs is proposed to conquer the challenges in HEM catalyst fabrications and applications.

关键词: high-entropy     electrocatalysis     synthetic methods     water-electrolysis     hydrogen and oxygen evolutions    

Oxygen-deficient MoO/NiS heterostructure grown on nickel foam as efficient and durable self-supportedelectrocatalysts for hydrogen evolution reaction

《化学科学与工程前沿(英文)》 2023年 第17卷 第4期   页码 437-448 doi: 10.1007/s11705-022-2228-1

摘要: High-performance and ultra-durable electrocatalysts are vital for hydrogen evolution reaction (HER) during water splitting. Herein, by one-pot solvothermal method, MoOx/Ni3S2 spheres comprising Ni3S2 nanoparticles inside and oxygen-deficient amorphous MoOx outside in situ grow on Ni foam (NF), to assembly the heterostructure composites of MoOx/Ni3S2/NF. By adjusting volume ratio of the solvents of ethanol to water, the optimized MoOx/Ni3S2/NF-11 exhibits the best HER performance, requiring an extremely low overpotential of 76 mV to achieve the current density of 10 mA∙cm‒2 (η10 = 76 mV) and an ultra-small Tafel slope of 46 mV∙dec‒1 in 0.5 mol∙L‒1 H2SO4. More importantly, the catalyst shows prominent high catalytic stability for HER (> 100 h). The acid-resistant MoOx wraps the inside Ni3S2/NF to ensure the high stability of the catalyst under acidic conditions. Density functional theory calculations confirm that the existing oxygen vacancy and MoOx/Ni3S2 heterostructure are both beneficial to the reduced Gibbs free energy of hydrogen adsorption (|∆GH*|) over Mo sites, which act as main active sites. The heterostructure effectively decreases the formation energy of O vacancy, leading to surface reconstruction of the catalyst, further improving HER performance. The MoOx/Ni3S2/NF is promising to serve as a highly effective and durable electrocatalyst toward HER.

关键词: molybdenum oxides     oxygen vacancies     heterostructure     electrocatalysts     hydrogen evolution reaction    

Energy distribution between liquid hydrogen and liquid oxygen temperatures in a Stirling/pulse tube refrigerator

《能源前沿(英文)》 2023年 第17卷 第4期   页码 516-526 doi: 10.1007/s11708-022-0844-6

摘要: A two-stage gas-coupled Stirling/pulse tube refrigerator (SPR), whose first and second stages respectively involve Stirling and pulse tube refrigeration cycles, is a very promising spaceborne refrigerator. The SPR has many advantages, such as a compact structure, high reliability, and high performance, and is expected to become an essential refrigerator for space applications. In research regarding gas-coupled regenerative refrigerator, the energy flow distribution between the two stages, and optimal phase difference between the pressure wave and volume flow, are two critical parameters that could widely influence refrigerator performance. The effects of displacer displacement on the pressure wave, phase difference, acoustic power distribution, and inter-stage cooling capacity shift of the SPR have been investigated experimentally. Notably, to obtain the maximum first-stage cooling capacity, an inflection point in displacement exists. When the displacer displacement is larger than the inflection point, the cooling capacity could be distributed between the first and second stages. In the present study, an SPR was designed and manufactured to work between the liquid hydrogen and liquid oxygen temperatures, which can be used to cool small-scale zero boil-off systems and space detectors. Under appropriate displacer displacement, the SPR can reach a no-load cooling temperature of 15.4 K and obtain 2.6 W cooling capacity at 70 K plus 0.1 W cooling capacity at 20 K with 160 W compressor input electric power.

关键词: Stirling/pulse tube refrigerator     displacer displacement     space application     phase shift     energy distribution    

nanosheets supported on N-doped carbon coated Ni foam as a highly active bifunctional electrocatalyst for hydrogenand oxygen evolution reactions

Miaomiao Tong, Lei Wang, Peng Yu, Xu Liu, Honggang Fu

《化学科学与工程前沿(英文)》 2018年 第12卷 第3期   页码 417-424 doi: 10.1007/s11705-018-1711-1

摘要:

A highly active bi-functional electrocatalyst towards both hydrogen and oxygen evolution reactions is critical for the water splitting. Herein, a self-supported electrode composed of 3D network nanostructured NiCoP nanosheets grown on N-doped carbon coated Ni foam (NiCoP/NF@NC) has been synthesized by a hydrothermal route and a subsequent phosphorization process. As a bifunctional electrocatalyst, the NiCoP/NF@NC electrode needs overpotentials of 31.8 mV for hydrogen evolution reaction and 308.2 mV for oxygen evolution reaction to achieve the current density of 10 mA·cm2 in 1 mol·L1 KOH electrolyte. This is much better than the corresponding monometal catalysts of CoP/NF@NC and NiP/NF@NC owing to the synergistic effect. NiCoP/NF@NC also exhibits low Tafel slope, and excellent long-term stability, which are comparable to the commercial noble catalysts of Pt/C and RuO2.

关键词: bimetallic phosphides     N-doped carbon     self-support     hydrogen evolution     oxygen evolution    

Highly effective visible-photocatalytic hydrogen evolution and simultaneous organic pollutant degradationover an urchin-like oxygen-doped MoS/ZnInS composite

《环境科学与工程前沿(英文)》 2022年 第16卷 第10期 doi: 10.1007/s11783-022-1566-z

摘要:

● An urchin-like OMS/ZIS composite was fabricated by a facile solvothermal method.

关键词: Dual-functional photocatalysts     Oxygen-doped MoS2/ZnIn2S4     H2 evolution     Organic pollutant    

Removal of dissolved oxygen from water using a Pd-resin based catalytic reactor

Wenxin SHI, Chongwei CUI, Liye ZHAO, Shuili YU, Xia YUN

《化学科学与工程前沿(英文)》 2009年 第3卷 第1期   页码 107-111 doi: 10.1007/s11705-009-0154-0

摘要: The removal of dissolved oxygen (DO) from water was studied experimentally in a Pd-resin base catalyst reactor using purified hydrogen gas as a reducing agent. The effects of various operating conditions, such as hydrogen and water flow rates, height of the catalytic resin bed, temperature, pH value and run time, on the removal of DO, had been studied extensively. The results shows that DO could be removed by the reactor from ppm to ppb levels at ambient temperature. Increases of temperature, H gas rate and the height of the catalytic resin were helpful to improve the DO removal rate. The change of pH value from 4 to 12 resulted in no effect on DO removal. Reaction time was the key factor to control the DO removal efficiency. Only when the reaction time was longer than 2.3 minutes under the experimental conditions, could a very low DO level be achieved.

关键词: dissolved oxygen     palladium     catalytic reactor     hydrogen     resin    

海上风电开发与多能源协同供电规模化制氢(氧)产业基地建设研究

金春鹏

《中国工程科学》 2015年 第17卷 第3期   页码 56-59

摘要:

中国风能资源丰富,沿海尤其是近海海域风能资源更为丰富,为大规模、超大规模海上风电发展创造了巨大空间。大规模非并网风电的应用,更是开辟了一条中国特色风电多元化发展之路。本文分析了海上风能资源布局及沿海风电开发现状;在风电非并网理论指导下,以规模化制氢产业为例,探讨非并网风电与高载能产业间的链合路径,并构建相应产业链;依据产业链合机制,探讨多能源协同供电规模化制氢(氧)产业基地建设的实施目标与战略规划。

关键词: 海上风电;多能源协同供电;规模化制氢(氧);产业基地    

Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient multifunctional electrocatalysts

《化学科学与工程前沿(英文)》 2021年 第15卷 第6期   页码 1487-1499 doi: 10.1007/s11705-021-2085-3

摘要: Developing cost-effective electrocatalysts for oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is vital in energy conversion and storage applications. Herein, we report a simple method for the synthesis of graphene-reinforced CoS/C nanocomposites and the evaluation of their electrocatalytic performance for typical electrocatalytic reactions. Nanocomposites of CoS embedded in N, S co-doped porous carbon and graphene (CoS@C/Graphene) were generated via simultaneous sulfurization and carbonization of one-pot synthesized graphite oxide-ZIF-67 precursors. The obtained CoS@C/Graphene nanocomposites were characterized by X-ray diffraction, Raman spectroscopy, thermogravimetric analysis-mass spectroscopy, scanning electronic microscopy, transmission electronic microscopy, X-ray photoelectron spectroscopy and gas sorption. It is found that CoS nanoparticles homogenously dispersed in the in situ formed N, S co-doped porous carbon/graphene matrix. The CoS@C/10Graphene composite not only shows excellent electrocatalytic activity toward ORR with high onset potential of 0.89 V, four-electron pathway and superior durability of maintaining 98% of current after continuously running for around 5 h, but also exhibits good performance for OER and HER, due to the improved electrical conductivity, increased catalytic active sites and connectivity between the electrocatalytic active CoS and the carbon matrix. This work offers a new approach for the development of novel multifunctional nanocomposites for the next generation of energy conversion and storage applications.

关键词: MOF derivative     graphene     electrocatalyst     oxygen reduction reaction     oxygen evolution reaction     hydrogen evolution reaction    

Evaluation of the technoeconomic feasibility of electrochemical hydrogen peroxide production for decentralized

Yang Li, Yixin Zhang, Guangshen Xia, Juhong Zhan, Gang Yu, Yujue Wang

《环境科学与工程前沿(英文)》 2021年 第15卷 第1期 doi: 10.1007/s11783-020-1293-2

摘要: Abstract • Gas diffusion electrode (GDE) is a suitable setup for practical water treatment. • Electrochemical H2O2 production is an economically competitive technology. • High current efficiency of H2O2 production was obtained with GDE at 5–400 mA/cm2. • GDE maintained high stability for H2O2 production for ~1000 h. • Electro-generation of H2O2 enhances ibuprofen removal in an E-peroxone process. This study evaluated the feasibility of electrochemical hydrogen peroxide (H2O2) production with gas diffusion electrode (GDE) for decentralized water treatment. Carbon black-polytetrafluoroethylene GDEs were prepared and tested in a continuous flow electrochemical cell for H2O2 production from oxygen reduction. Results showed that because of the effective oxygen transfer in GDEs, the electrode maintained high apparent current efficiencies (ACEs,>80%) for H2O2 production over a wide current density range of 5–400 mA/cm2, and H2O2 production rates as high as ~202 mg/h/cm2 could be obtained. Long-term stability test showed that the GDE maintained high ACEs (>85%) and low energy consumption (<10 kWh/kg H2O2) for H2O2 production for 42 d (~1000 h). However, the ACEs then decreased to ~70% in the following 4 days because water flooding of GDE pores considerably impeded oxygen transport at the late stage of the trial. Based on an electrode lifetime of 46 days, the overall cost for H2O2 production was estimated to be ~0.88 $/kg H2O2, including an electricity cost of 0.61 $/kg and an electrode capital cost of 0.27 $/kg. With a 9 cm2 GDE and 40 mA/cm2 current density, ~2–4 mg/L of H2O2 could be produced on site for the electro-peroxone treatment of a 1.2 m3/d groundwater flow, which considerably enhanced ibuprofen abatement compared with ozonation alone (~43%–59% vs. 7%). These findings suggest that electrochemical H2O2 production with GDEs holds great promise for the development of compact treatment technologies for decentralized water treatment at a household and community level.

关键词: Advanced oxidation process     Electro-peroxone     Gas diffusion electrode     Hydrogen peroxide     Oxygen reduction    

An overview and recent advances in electrocatalysts for direct seawater splitting

《化学科学与工程前沿(英文)》 2021年 第15卷 第6期   页码 1408-1426 doi: 10.1007/s11705-021-2102-6

摘要: In comparison to pure water, seawater is widely accepted as an unlimited resource. The direct seawater splitting is economical and eco-friendly, but the key challenges in seawater, especially the chlorine-related competing reactions at the anode, seriously hamper its practical application. The development of earth-abundant electrocatalysts toward direct seawater splitting has emerged as a promising strategy. Highly efficient electrocatalysts with improved selectivity and stability are of significance in preventing the interference of side reactions and resisting various impurities. This review first discusses the macroscopic understanding of direct seawater electrolysis and then focuses on the strategies for rational design of electrocatalysts toward direct seawater splitting. The perspectives of improved electrocatalysts to solve emerging challenges and further development of direct seawater splitting are also provided.

关键词: seawater splitting     electrocatalysts     oxygen evolution reaction     hydrogen evolution reaction     chlorine chemistry    

Speciation evolutions of target metals (Cd, Pb) influenced by chlorine and sulfur during sewage sludge

Jingde LUAN,Rundong LI,Zhihui ZHANG,Yanlong LI,Yun ZHAO

《环境科学与工程前沿(英文)》 2014年 第8卷 第6期   页码 871-876 doi: 10.1007/s11783-013-0621-1

摘要: In sludge incineration, the thermal behavior of heavy metal is a growing concern. In this work, the combined analysis of metal partitioning behavior between vapor phase and condensed phase, speciation redistribution in condensed phase and the difference of metal species in binding energy was carried out to investigate the possible volatilization-condensation mechanism of heavy metals in high-temperature sludge incineration. It was found that there were two steps in metal volatilization. The initial volatilization of heavy metal originated from their exchangeable (EXC), carbonate bound (CAR) and iron–manganese bound (FM) fractions, which is primarily composed of simple substance, chlorides, oxides and sulfides. With the increase of chlorine and sulfur in sludge, the inner speciation redistribution of heavy metals occurred in condensed phase, which was an important factor affecting the potential volatility of heavy metals. A partial of metal species with complexed (COM) and residual (RES) fractions gradually decomposed into simple substance or ions, oxides and carbonates, which significantly strengthened the second volatility. In presence of chlorine, about 46% of Cd with the RES fraction disappeared when the volatility rate of Cd increased by 44.89%. Moreover, about 9% of Pb with COM fraction disappeared when there was an increase of nearly 10% in the volatilization rate. Thus, the second volatilization was mainly controlled by the decomposition of metal species with COM and RES fractions. By virtue of XRD analysis and the binding energy calculation, it was found that metal complex and silicates were inclined to decompose under high temperature due to poor thermo stability as compared with sulfates.

关键词: sludge incineration     heavy metals     inner speciation redistribution     binding energy    

Preparation of ceria-zirconia solid solution with enhanced oxygen storage capacity and redox performance

Lijing MENG, Licheng LIU, Xuehong ZI, Hongxing DAI, Hong HE, Zhen ZHAO, Xinping WANG,

《环境科学与工程前沿(英文)》 2010年 第4卷 第2期   页码 164-171 doi: 10.1007/s11783-010-0019-2

摘要: A new method called ultrasonic-assisted membrane reaction (UAMR) was reported for the fabrication of ceria-zirconia solid solution. A series of ceria-zirconia solid solutions with different Ce/Zr molar ratios were prepared by the UAMR method and characterized by X-ray diffraction (XRD), N adsorption, hydrogen temperature-programmed reduction (H-TPR), scanning electron microscope (SEM), and transmission electron microscopy (TEM) techniques. The UAMR method proved to be superior, especially when the Ce/Zr molar ratio was lower than 1, in fabricating ceria-zirconia solid solutions with large BET surface area, high oxygen storage capacity (OSC), and low reduction temperature.

关键词: membrane reaction     ceria-zirconia     Ce/Zr molar ratio     solid solution     hydrogen temperature-programmed reduction (H2-TPR)    

Facile route to achieve MoSe-NiSe on nickel foam as efficient dual functional electrocatalysts for overall water splitting

《能源前沿(英文)》 2022年 第16卷 第3期   页码 483-491 doi: 10.1007/s11708-022-0813-0

摘要: Since the catalytic activity of present nickel-based synthetic selenide is still to be improved, MoSe2-Ni3Se2 was synthesized on nickel foam (NF) (MoSe2-Ni3Se2/NF) by introducing a molybdenum source. After the molybdenum source was introduced, the surface of the catalyst changed from a single-phase structure to a multi-phase structure. The catalyst surface with enriched active sites and the synergistic effect of MoSe2 and Ni3Se2 together enhance the hydrogen evolution reactions (HER), the oxygen evolution reactions (OER), and electrocatalytic total water splitting activity of the catalyst. The overpotential of the MoSe2-Ni3Se2/NF electrocatalyst is only 259 mV and 395 mV at a current density of 100 mA/cm2 for HER and OER, respectively. MoSe2-Ni3Se2/NF with a two-electrode system attains a current density of 10 mA/cm2 at 1.60 V. In addition, the overpotential of HER and OER of MoSe2-Ni3Se2/NF within 80000 s and the decomposition voltage of electrocatalytic total water decomposition hardly changed, showing an extremely strong stability. The improvement of MoSe2-Ni3Se2/NF catalytic activity is attributed to the establishment of the multi-phase structure and the optimized inoculation of the multi-component and multi-interface.

关键词: three-dimensional molybdenum nanomaterials     hydrogen evolution reaction     oxygen evolution reaction     overall water splitting    

Simultaneous CO

Jie ZHU,Wei WANG,Xiuning HUA,Zhou XIA,Zhou DENG

《环境科学与工程前沿(英文)》 2015年 第9卷 第6期   页码 1117-1129 doi: 10.1007/s11783-015-0812-z

摘要: The chemical looping concept provided a novel way to achieve carbon separation during the production of energy or substances. In this work, hydrogen generation with inherent CO capture in single packed bed reactor via this concept was discussed. Two oxygen carriers, Fe O 60 wt.% and Fe O 55 wt.%/CuO 5 wt.% supported by Al O , were made by ball milling method. First, according to the characteristics of the reduction breakthrough curve, a strict fuel supply strategy was selected to achieve simultaneous CO capture and H production. Then, in the long term tests using CO as fuel, it was proved that CuO addition improved hydrogen generation with the maximum intensity of 3700 μmol H ·g Fe O compared with Fe-Al of 2300 μmol H ·g Fe O . The overall CO capture efficiency remained 98%–98.8% over 100 cycles. Moreover, the reactivity of deactivated materials was recovered nearly like that of fresh ones by sintering treatment. Finally, two kinds of complex gases consist of CO, H , CH and CO were utilized as fuels to test the feasibility. The results showed all components could be completely converted by Fe-Cu-Al in the reduction stage. The intensity of hydrogen production and the overall CO capture efficiency were in the range of 2000–2400 μmol H ·g Fe O and 89%–95%, respectively.

关键词: CO2 capture     chemical looping hydrogen generation     iron based oxygen carriers     single packed bed reactor     long-term test     complex gases fuel    

Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reductionand oxygen evolution reaction: a density functional theory study

《化学科学与工程前沿(英文)》 2023年 第17卷 第5期   页码 570-580 doi: 10.1007/s11705-022-2247-y

摘要: Recently, metal–organic frameworks are one of the potential catalytic materials for electrocatalytic applications. The oxygen reduction reaction and oxygen evolution reaction catalytic activities of heterometallic cluster-based organic frameworks are investigated using density functional theory. Firstly, the catalytic activities of heterometallic clusters are investigated. Among all heterometallic clusters, Fe2Mn–Mn has a minimum overpotential of 0.35 V for oxygen reduction reaction, and Fe2Co–Co possesses the smallest overpotential of 0.32 V for oxygen evolution reaction, respectively 100 and 50 mV lower than those of Pt(111) and RuO2(110) catalysts. The analysis of the potential gap of Fe2M clusters indicates that Fe2Mn, Fe2Co, and Fe2Ni clusters possess good bifunctional catalytic activity. Additionally, the catalytic activity of Fe2Mn and Fe2Co connected through 3,3′,5,5′-azobenzenetetracarboxylate linker to form Fe2M–PCN–Fe2M is explored. Compared with Fe2Mn–PCN–Fe2Mn, Fe2Co–PCN–Fe2Co, and isolated Fe2M clusters, the mixed-metal Fe2Co–PCN–Fe2Mn possesses excellent bifunctional catalytic activity, and the values of potential gap on the Mn and Co sites of Fe2Co–PCN–Fe2Mn are 0.69 and 0.70 V, respectively. Furthermore, the analysis of the electron structure indicates that constructing a mixed-metal cluster can efficiently enhance the electronic properties of the catalyst. In conclusion, the mixed-metal cluster strategy provides a new approach to further design and synthesize high-efficiency bifunctional electrocatalysts.

关键词: bimetallic metal–organic frameworks     bifunctional electrocatalyst     density functional theory     oxygen reduction reaction     oxygen evolution reaction    

标题 作者 时间 类型 操作

High-entropy catalysts for electrochemical water-electrolysis of hydrogen evolution and oxygen evolution

期刊论文

Oxygen-deficient MoO/NiS heterostructure grown on nickel foam as efficient and durable self-supportedelectrocatalysts for hydrogen evolution reaction

期刊论文

Energy distribution between liquid hydrogen and liquid oxygen temperatures in a Stirling/pulse tube refrigerator

期刊论文

nanosheets supported on N-doped carbon coated Ni foam as a highly active bifunctional electrocatalyst for hydrogenand oxygen evolution reactions

Miaomiao Tong, Lei Wang, Peng Yu, Xu Liu, Honggang Fu

期刊论文

Highly effective visible-photocatalytic hydrogen evolution and simultaneous organic pollutant degradationover an urchin-like oxygen-doped MoS/ZnInS composite

期刊论文

Removal of dissolved oxygen from water using a Pd-resin based catalytic reactor

Wenxin SHI, Chongwei CUI, Liye ZHAO, Shuili YU, Xia YUN

期刊论文

海上风电开发与多能源协同供电规模化制氢(氧)产业基地建设研究

金春鹏

期刊论文

Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient multifunctional electrocatalysts

期刊论文

Evaluation of the technoeconomic feasibility of electrochemical hydrogen peroxide production for decentralized

Yang Li, Yixin Zhang, Guangshen Xia, Juhong Zhan, Gang Yu, Yujue Wang

期刊论文

An overview and recent advances in electrocatalysts for direct seawater splitting

期刊论文

Speciation evolutions of target metals (Cd, Pb) influenced by chlorine and sulfur during sewage sludge

Jingde LUAN,Rundong LI,Zhihui ZHANG,Yanlong LI,Yun ZHAO

期刊论文

Preparation of ceria-zirconia solid solution with enhanced oxygen storage capacity and redox performance

Lijing MENG, Licheng LIU, Xuehong ZI, Hongxing DAI, Hong HE, Zhen ZHAO, Xinping WANG,

期刊论文

Facile route to achieve MoSe-NiSe on nickel foam as efficient dual functional electrocatalysts for overall water splitting

期刊论文

Simultaneous CO

Jie ZHU,Wei WANG,Xiuning HUA,Zhou XIA,Zhou DENG

期刊论文

Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reductionand oxygen evolution reaction: a density functional theory study

期刊论文