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Hollow carbon spheres and their noble metal-free hybrids in catalysis

《化学科学与工程前沿（英文）》 2021年第15卷第6期页码 1380-1407 doi: 10.1007/s11705-021-2097-z

摘要： Hollow carbon spheres have garnered great interest owing to their high surface area, large surface-to-volume ratio and reduced transmission lengths. Herein, we overview hollow carbon sphere-based materials and their noble metal-free hybrids in catalysis. Firstly, we summarize the key fabrication techniques for various kinds of hollow carbon spheres, with a particular emphasis on controlling pore structure and surface morphology, and then heterogeneous doping as well as their metal-free/containing hybrids are presented; next, possible applications for non-noble metal/hollow carbon sphere hybrids in the area of energy-related catalysis, including oxygen reduction reaction, hydrogen evolution reaction, oxygen evolution reaction, water splitting, rechargeable Zn-air batteries and pollutant degradation are discussed; finally, we introduce the various challenges and opportunities offered by hollow carbon spheres from the perspective of synthesis and catalysis.

关键词： hollow carbon spheres functionalization noble metal-free catalysis

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Copper nanoparticles/polyaniline-derived mesoporous carbon electrocatalysts for hydrazine oxidation

Tao Zhang, Tewodros Asefa

《化学科学与工程前沿（英文）》 2018年第12卷第3期页码 329-338 doi: 10.1007/s11705-018-1741-8

摘要：

Copper nanoparticles-decorated polyaniline-derived mesoporous carbon that can serve as noble metal-free electrocatalyst for the hydrazine oxidation reaction (HzOR) is synthesized via a facile synthetic route. The material exhibits excellent electrocatalytic activity toward HzOR with low overpotential and high current density. The material also remains stable during the electrocatalytic reaction for long time. Its good electrocatalytic performance makes this material a promising alternative to conventional noble metal-based catalysts (e.g., Pt) that are commonly used in HzOR-based fuel cells.

关键词： copper nanoparticles mesoporous carbon noble metal-free electrocatalyst hydrazine oxidation reaction polyaniline

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Recent advances on metal-free graphene-based catalysts for the production of industrial chemicals

Zhiyong Wang, Yuan Pu, Dan Wang, Jie-Xin Wang, Jian-Feng Chen

《化学科学与工程前沿（英文）》 2018年第12卷第4期页码 855-866 doi: 10.1007/s11705-018-1722-y

摘要： With the development of carbon catalysts, graphene-based metal-free catalysts have drawn increasing attention in both scientific research and in industrial chemical production processes. In recent years, the catalytic activities of metal-free catalysts have significantly improved and they have become promising alternatives to traditional metal-based catalysts. The use of metal-free catalysts greatly improves the sustainability of chemical processes. In view of this, the recent progress in the preparation of graphene-based metal-free catalysts along with their applications in catalytic oxidation, reduction and coupling reactions are summarized in this review. The future trends and challenges for the design of graphene-based materials for industrial organic catalytic reactions with good stabilities and high catalytic performance are also discussed.

关键词： graphene-based materials metal-free catalyst industrial chemical productions catalytic reaction

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Metal-free, carbon-based catalysts for oxygen reduction reactions

Zhiyi Wu,Zafar Iqbal,Xianqin Wang

《化学科学与工程前沿（英文）》 2015年第9卷第3期页码 280-294 doi: 10.1007/s11705-015-1524-4

摘要： Developing metal-free, carbon-based catalysts to replace platinum-based catalysts for oxygen reduction reactions (ORRs) is an emerging area of research. In recent years, different carbon structures including carbon doped with IIIA-VIIA heteroatoms (C−M site-based, where M represents the doped heteroatom) and polynitrogen (PN) compounds encapsulated in carbon nanotubes (CNTs) (N−N site-based) have been synthesized. Compared to metallic catalysts, these materials are highly active, stable, inexpensive, and environmentally friendly. This review discusses the development of these materials, their ORR performances and the mechanisms for how the incorporation of heteroatoms enhances the ORR activity. Strategies for tailoring the structures of the carbon substrates to improve ORR performance are also discussed. Future studies in this area will need to include optimizing synthetic strategies to control the type, amount and distribution of the incorporated heteroatoms, as well as better understanding the ORR mechanisms in these catalysts.

关键词： oxygen reduction reaction electrocatalysis metal-free carbon-based polynitrogen

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Noble-metal-free cobalt hydroxide nanosheets for efficient electrocatalytic oxidation

Jie Lan, Daizong Qi, Jie Song, Peng Liu, Yi Liu, Yun-Xiang Pan

《化学科学与工程前沿（英文）》 2020年第14卷第6期页码 948-955 doi: 10.1007/s11705-020-1920-2

摘要： Cobalt hydroxide has been emerging as a promising catalyst for the electrocatalytic oxidation reactions, including the oxygen evolution reaction (OER) and glucose oxidation reaction (GOR). Herein, we prepared cobalt hydroxide nanoparticles (CoHP) and cobalt hydroxide nanosheets (CoHS) on nickel foam. In the electrocatalytic OER, CoHS shows an overpotential of 306 mV at a current density of 10 mA·cm . This is enhanced as compared with that of CoHP (367 mV at 10 mA·cm ). In addition, CoHS also exhibits an improved performance in the electrocatalytic GOR. The improved electrocatalytic performance of CoHS could be due to the higher ability of the two-dimensional nanosheets on CoHS in electron transfer. These results are useful for fabricating efficient catalysts for electrocatalytic oxidation reactions.

关键词： electrocatalytic oxidation cobalt hydroxide nanosheet water glucose

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超重力环境下非金属氮掺杂石墨烯泡沫催化还原反应性能研究 Article

王志勇, 赵志建, Jesse Baucom, 王丹, Liming Dai, 陈建峰

《工程（英文）》 2020年第6卷第6期页码 680-687 doi: 10.1016/j.eng.2019.12.018

摘要：

本文以硝基苯还原和亚甲基蓝降解为模型反应体系，以非金属氮掺杂石墨烯泡沫（NGF）作为三维结构式催化材料，研究了超重力环境对催化反应性能的影响。在超重力旋转圆管反应器内6484 g (g = 9.81 m·s^–2)的超重力环境下，非金属催化硝基苯还原的表观速率常数是传统搅拌反应器内的6 倍。通过计算流体力学理论模拟，揭示了超重力旋转管式反应器内超重力水平较高，湍流动能比传统反应器内有显著提高，液固相表面更新速度快，提高了催化反应效率。X射线光电子能谱和拉曼光谱测试表明该催化材料组成和结构在超重力环境下的反应过程中保持稳定。在另一个模型反应体系中，非金属氮掺杂石墨烯泡沫催化亚甲基蓝降解的速率也随着超重力水平的增加而增大。这些结果表明了超重力强化非金属碳基催化材料催化还原反应的潜力。

关键词：超重力技术过程强化非金属催化碳基纳米材料催化还原

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Effect of noble metal nanoparticle size on C–N bond cleavage performance in hydrodenitrogenation: a study

《化学科学与工程前沿（英文）》 2023年第17卷第12期页码 1986-2000 doi: 10.1007/s11705-023-2337-5

摘要： Breakage of the C–N bond is a structure sensitive process, and the catalyst size significantly affects its activity. On the active metal nanoparticle scale, the role of catalyst size in C–N bond cleavage has not been clearly elucidated. So, Ru catalysts with variable nanoparticle sizes were obtained by modulating the reduction temperature, and the catalytic activity was evaluated using 1,2,3,4-tetrahydroquinoline and o-propylaniline with different C–N bond hybridization patterns as reactants. Results showed a 13 times higher reaction rate for sp³-hybridized C–N bond cleavage than sp²-hybridized C–N bond cleavage, while the reaction rate tended to increase first and then decrease as the catalyst nanoparticle size increased. Different concentrations of terrace, step, and corner sites were found in different sizes of Ru nanoparticles. The relationship between catalytic site variation and C–N bond cleavage activity was further investigated by calculating the turnover frequency values for each site. This analysis indicates that the variation of different sites on the catalyst is the intrinsic factor of the size dependence of C–N bond cleavage activity, and the step atoms are the active sites for the C–N bond cleavage. When Ru nanoparticles are smaller than 1.9 nm, they have a strong adsorption effect on the reactants, which will affect the catalytic performance of the Ru catalyst. Furthermore, these findings were also confirmed on other metallic Pd/Pt catalysts. The role of step sites in C–N bond cleavage was proposed using the density function theory calculations. The reactants have stronger adsorption energies on the step atoms, and step atoms have d-band center nearer to the Fermi level. In this case, the interaction with the reactant is stronger, which is beneficial for activating the C–N bond of the reactant.

关键词： sp³/sp²-hybridized C–N bond noble metal nanoparticle catalytic active site turnover frequency DFT

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Shape/size controlling syntheses, properties and applications of two-dimensional noble metal nanocrystals

Baozhen An,Mingjie Li,Jialin Wang,Chaoxu Li

《化学科学与工程前沿（英文）》 2016年第10卷第3期页码 360-382 doi: 10.1007/s11705-016-1576-0

摘要： Two dimensional (2D) nanocrystals of noble metals (e.g., Au, Ag, Pt) often have unique structural and environmental properties which make them useful for applications in electronics, optics, sensors and biomedicines. In recent years, there has been a focus on discovering the fundamental mechanisms which govern the synthesis of the diverse geometries of these 2D metal nanocrystals (e.g., shapes, thickness, and lateral sizes). This has resulted in being able to better control the properties of these 2D structures for specific applications. In this review, a brief historical survey of the intrinsic anisotropic properties and quantum size effects of 2D noble metal nanocrystals is given and then a summary of synthetic approaches to control their shapes and sizes is presented. The unique properties and fascinating applications of these nanocrystals are also discussed.

关键词： two-dimension noble metal nanocrystal surface plasmon controllable synthesis

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Catalytic activity of noble metal nanoparticles toward hydrodechlorination: influence of catalyst electronic

Man ZHANG,Feng HE,Dongye ZHAO

《环境科学与工程前沿（英文）》 2015年第9卷第5期页码 888-896 doi: 10.1007/s11783-015-0774-1

摘要： In this study, stabilized Pd, Pt and Au nanoparticles were successfully prepared in aqueous phase using sodium carboxymethyl cellulose (CMC) as a capping agent. These metal nanoparticles were then tested for catalytic hydrodechlorination toward two classes of organochlorinated compounds (vinyl polychlorides including trichloroethylene (TCE), tetrachloroethylene (PCE), and alkyl polychlorides including 1,1,1-trichloroethane (1,1,1-TCA), and 1,1,1,2-tetrachloroethane (1,1,1,2-TeCA)) to determine the rate-limiting steps and to explore the reaction mechanisms. The surface area normalized reaction rate constant, , showed a systematic dependence on the electronic structure (the density of states at the Fermi level) of the metals, suggesting that adsorption of organochlorinated reactants on the metal catalyst surfaces is the rate-limiting step for catalytic hydrodechlorination. Hydrodechlorination rates of 1,1,1-TCA and 1,1,1,2-TeCA agreed with the bond strength of the first (weakest) dissociated C-Cl bond, suggesting that C-Cl bond cleavage, which is the first step for dissociative adsorption of the alkyl polychlorides, controlled the catalytic hydrodechlorination rate. However, hydrodechlorination rates of TCE and PCE correlated with the adsorption energies of their molecular (non-dissociative) adsorption on the noble metals rather than with the first C-Cl bond strength, suggesting that molecular adsorption governs the reaction rate for hydrodechlorination of the vinyl polychlorides.

关键词： catalytic hydrodechlorination electronic structure metal nanoparticles reaction mechanisms

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以NH₃OH⁺/NH₂NH₃⁺作为B位阳离子的无金属六方钙钛矿含能材料 Article

尚宇, 余志鸿, 黄瑞康, 陈劭力, 刘德轩, 陈晓娴, 张伟雄, 陈小明

《工程（英文）》 2020年第6卷第9期页码 1013-1018 doi: 10.1016/j.eng.2020.05.018

摘要：

寻找可经由简单路线合成的高性能含能材料是发展先进实用含能材料的重要问题。文中通过合理地选择分子组分，经由易于规模放大的简单合成路线，以NH₃OH⁺和NH₂NH₃⁺分别作为B位点阳离子构筑了两例无金属六方钙钛矿含能材料(H₂dabco)B(ClO₄)₃（分别命名为DAP-6和DAP-7，其中H₂dabco²⁺是1,4-二氮杂双环[2.2.2]辛烷-1,4-二鎓离子）。与基于NH₄⁺阳离子构筑的立方钙钛矿类似物(H₂dabco)(NH₄)(ClO₄)₃相比，DAP-6和DAP-7有较高的晶体堆积密度和生成焓，从而具有更高的爆轰性能。特别地，DAP-7具有超高热稳定性（起始分解温度T_d = 375.3 °C）、高爆速（D = 8.883 km·s^‒1）和高爆压（P = 35.8 GPa），因此具有作为耐热炸药的应用潜力。计算表明，DAP-6不仅具有较高的热稳定性（T_d = 245.9 °C）以及优异的爆轰性能（D = 9.123 km·s^‒1，P = 38.1 GPa），而且其爆热值（Q = 6.35 kJ·g^‒1）和理论比冲值（I_sp= 265.3 s）均稍优于六硝基六氮杂异伍兹烷（CL-20：Q = 6.23 kJ·g^‒1，I_sp = 264.8 s），在炸药和推进剂领域中具有很好的应用前景。

关键词：含能材料单质炸药固体推进剂无金属六方钙钛矿

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Sulfur-deficient CoNi₂S₄ nanoparticles-anchored porous carbon nanofibers as bifunctional electrocatalyst

《化学科学与工程前沿（英文）》 2023年第17卷第11期页码 1707-1717 doi: 10.1007/s11705-023-2308-x

摘要： Water electrolysis technology is considered to be one of the most promising means to produce hydrogen. Herein, aiming at the problems of high overpotential and slow kinetics in water splitting, N-doped porous carbon nanofibers-coupled CoNi₂S₄ nanoparticles are prepared as bifunctional electrocatalyst. In the strategy, NaCl is used as the template to prepare porous carbon nanofibers with a large surface area, and sulfur vacancies are created to modulate the electronic structure of CoNi₂S₄. Electron spin resonance confirms the formation of abundant sulfur vacancies, which largely reduce the bandgap of CoNi₂S₄ from 1.68 to 0.52 eV. The narrowed bandgap is conducive to the migration of valence electrons and decreases the charge transfer resistance for electrocatalytic reaction. Moreover, the uniform distribution of CoNi₂S₄ nanoparticles on carbon nanofibers can prevent the aggregation and facilitate the exposure of electrochemical active sites. Therefore, the composite catalyst exhibits low overpotentials of 340 mV@100 mA·cm^–2 for oxygen evolution reaction and 380 mV@100 mA·cm^–2 for hydrogen evolution reaction. The assembled electrolyzer requires 1.64 V to achieve 10 mA·cm^–2 for overall water-splitting with good long-term stability. The excellent performance results from the synergistic effect of porous structures, sulfur deficiency, nitrogen doping, and the well-dispersed active component.

关键词： nanoparticle sulfur vacancy porous carbon nanofiber transition metal sulfides electrolysis

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

《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

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Zinc modification of Ni-Ti as efficient NiZnTi catalysts with both geometric and electronic improvements for hydrogenation of nitroaromatics

《化学科学与工程前沿（英文）》 2022年第16卷第4期页码 461-474 doi: 10.1007/s11705-021-2072-8

摘要： The catalytic hydrogenation of nitroaromatics is an environmentally friendly technology for aniline production, and it is crucial to develop noble-metal-free catalysts that can achieve chemoselective hydrogenation of nitroaromatics under mild reaction conditions. In this work, zinc-modified Ni-Ti catalysts (Ni_xZn_yTi₁) were fabricated and applied for the hydrogenation of nitroaromatics hydrogenation. It was found that the introduction of zinc effectively increases the surface Ni density, enhances the electronic effect, and improves the interaction between Ni and TiO₂, resulting in smaller Ni particle size, more oxygen vacancies, higher dispersion and greater concentration of Ni on the catalyst surface. Furthermore, the electron-rich Ni^δ^– obtained by electron transfer from Zn and Ti to Ni effectively adsorbs and dissociates hydrogen. The results reveal that Ni_xZn_yTi₁ (Ni_0.5Zn_0.5Ti₁) shows excellent catalytic performance under mild conditions (70 °C and 6 bar). These findings provide a rational strategy for the development of highly active non-noble-metal hydrogenation catalysts.

关键词： bimetal strategy oxygen vacancy non-noble metal catalyst hydrogenation aromatic nitro compounds

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Current challenge and perspective of PGM-free cathode catalysts for PEM fuel cells

Gang WU

《能源前沿（英文）》 2017年第11卷第3期页码 286-298 doi: 10.1007/s11708-017-0477-3

摘要： To significantly reduce the cost of proton exchange membrane fuel cells, platinum-group metal (PGM)-free cathode catalysts are highly desirable. Current M-N-C (M: Fe, Co or Mn) catalysts are considered the most promising due to their encouraging performance. The challenge thus has been their stability under acidic conditions, which has hindered their use for any practical applications. In this review, based on the author’s research experience in the field for more than 10 years, current challenges and possible solutions to overcome these problems were discussed. The current Edisonian approach (i.e., trial and error) to developing PGM-free catalysts has been ineffective in achieving revolutionary breakthroughs. Novel synthesis techniques based on a more methodological approach will enable atomic control and allow us to achieve optimal electronic and geometric structures for active sites uniformly dispersed within the 3D architectures. Structural and chemical controlled precursors such as metal-organic frameworks are highly desirable for making catalysts with an increased density of active sites and strengthening local bonding structures among N, C and metals. Advanced electrochemical and physical characterization, such as electron microscopy and X-ray absorption spectroscopy should be combined with first principle density functional theory (DFT) calculations to fully elucidate the active site structures.

关键词： oxygen reduction fuel cells cathode nonprecious metal catalysts carbon nanocomposites

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Heterometallic cluster-based organic frameworks as highly active electrocatalysts for oxygen reduction and 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

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标题作者时间类型操作

Hollow carbon spheres and their noble metal-free hybrids in catalysis

期刊论文

Copper nanoparticles/polyaniline-derived mesoporous carbon electrocatalysts for hydrazine oxidation

Tao Zhang, Tewodros Asefa

期刊论文

Recent advances on metal-free graphene-based catalysts for the production of industrial chemicals

Zhiyong Wang, Yuan Pu, Dan Wang, Jie-Xin Wang, Jian-Feng Chen

期刊论文

Metal-free, carbon-based catalysts for oxygen reduction reactions

Zhiyi Wu,Zafar Iqbal,Xianqin Wang

期刊论文

Noble-metal-free cobalt hydroxide nanosheets for efficient electrocatalytic oxidation

Jie Lan, Daizong Qi, Jie Song, Peng Liu, Yi Liu, Yun-Xiang Pan

期刊论文

超重力环境下非金属氮掺杂石墨烯泡沫催化还原反应性能研究

王志勇, 赵志建, Jesse Baucom, 王丹, Liming Dai, 陈建峰

期刊论文

Effect of noble metal nanoparticle size on C–N bond cleavage performance in hydrodenitrogenation: a study

期刊论文

Shape/size controlling syntheses, properties and applications of two-dimensional noble metal nanocrystals

Baozhen An,Mingjie Li,Jialin Wang,Chaoxu Li

期刊论文

Catalytic activity of noble metal nanoparticles toward hydrodechlorination: influence of catalyst electronic

Man ZHANG,Feng HE,Dongye ZHAO

期刊论文

以NH₃OH⁺/NH₂NH₃⁺作为B位阳离子的无金属六方钙钛矿含能材料

尚宇, 余志鸿, 黄瑞康, 陈劭力, 刘德轩, 陈晓娴, 张伟雄, 陈小明

期刊论文

Sulfur-deficient CoNi₂S₄ nanoparticles-anchored porous carbon nanofibers as bifunctional electrocatalyst

期刊论文

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

期刊论文

Zinc modification of Ni-Ti as efficient NiZnTi catalysts with both geometric and electronic improvements for hydrogenation of nitroaromatics

期刊论文

Current challenge and perspective of PGM-free cathode catalysts for PEM fuel cells

Gang WU

期刊论文

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

期刊论文

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