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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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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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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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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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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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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Td = 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（Td = 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（Isp = 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，Isp = 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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Rosin side chain type catalyst-free vitrimers with high cross-link density, mechanical strength, and

《化学科学与工程前沿（英文）》 2023年 第17卷 第9期   页码 1267-1279 doi: 10.1007/s11705-022-2291-7

摘要： The emergence of vitrimer, a new class of polymer materials can address the problem of recyclability, reprocess ability and recyclability of thermosetting plastics. Rosin, a natural product, is an ideal raw material for the preparation of polymers in a more sustainable way. Nevertheless, due to the huge steric hindrance caused by the hydrogenated phenanthrene ring structure, the cross-link density of materials is frequently lowered. In this study, hydrogenated rosin was adopted for preparing hydrogenated rosin side-chain type diacids, which were reacted with mixed epoxy to obtain rosin side-chain type vitrimers. It was completely characterized by differential scanning calorimetry test, thermogravimetric analysis, shape memory test and self-healing test. The prepared vitrimers exhibited good self-healing properties, excellent heat resistance (Td = 352 °C) as well as high mechanical properties (tensile strength of 46.75 MPa). The tricyclic diterpene structure of rosin was introduced into the side chain in order to avoid the reduction of cross-link density resulting from the huge steric hindrance of the rigid tricyclic hydrophenylene skeleton. Vitrimers can undergo dynamic transesterification reaction without external catalysts due to the autocatalytic effect of tertiary amines from epoxy. Moreover, our work expanded the application field of rosin, increased the added value of rosin, and provided a novel method for preparing rosin-based vitrimers with ideal properties.

关键词： vitrimers     rosin     catalyst-free     high mechanical properties     dynamic transesterification reaction    

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Exploration of the oxygen transport behavior in non-precious metal catalyst-based cathode catalyst layer

Shiqu CHEN, Silei XIANG, Zehao TAN, Huiyuan LI, Xiaohui YAN, Jiewei YIN, Shuiyun SHEN, Junliang ZHANG

《能源前沿（英文）》 2023年 第17卷 第1期   页码 123-133 doi: 10.1007/s11708-022-0849-1

摘要： High cost has undoubtedly become the biggest obstacle to the commercialization of proton exchange membrane fuel cells (PEMFCs), in which Pt-based catalysts employed in the cathodic catalyst layer (CCL) account for the major portion of the cost. Although non-precious metal catalysts (NPMCs) show appreciable activity and stability in the oxygen reduction reaction (ORR), the performance of fuel cells based on NPMCs remains unsatisfactory compared to those using Pt-based CCL. Therefore, most studies on NPMC-based fuel cells focus on developing highly active catalysts rather than facilitating oxygen transport. In this work, the oxygen transport behavior in CCLs based on highly active Fe-N-C catalysts is comprehensively explored through the elaborate design of two types of membrane electrode structures, one containing low-Pt-based CCL and NPMC-based dummy catalyst layer (DCL) and the other containing only the NPMC-based CCL. Using Zn-N-C based DCLs of different thickness, the bulk oxygen transport resistance at the unit thickness in NPMC-based CCL was quantified via the limiting current method combined with linear fitting analysis. Then, the local and bulk resistances in NPMC-based CCLs were quantified via the limiting current method and scanning electron microscopy, respectively. Results show that the ratios of local and bulk oxygen transport resistances in NPMC-based CCL are 80% and 20%, respectively, and that an enhancement of local oxygen transport is critical to greatly improve the performance of NPMC-based PEMFCs. Furthermore, the activity of active sites per unit in NPMC-based CCLs was determined to be lower than that in the Pt-based CCL, thus explaining worse cell performance of NPMC-based membrane electrode assemblys (MEAs). It is believed that the development of NPMC-based PEMFCs should proceed not only through the design of catalysts with higher activity but also through the improvement of oxygen transport in the CCL.

关键词： proton exchange membrane fuel cells (PEMFCs)     non-precious metal catalyst (NPMC)     cathode catalyst layer (CCL)     local and bulk oxygen transport resistance    

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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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Diffusion process in enzyme–metal hybrid catalysts

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 921-929 doi: 10.1007/s11705-022-2144-4

摘要： Enzyme–metal hybrid catalysts bridge the gap between enzymatic and heterogeneous catalysis, which is significant for expanding biocatalysis to a broader scope. Previous studies have demonstrated that the enzyme–metal hybrid catalysts exhibited considerably higher catalytic efficiency in cascade reactions, compared with that of the combination of separated enzyme and metal catalysts. However, the precise mechanism of this phenomenon remains unclear. Here, we investigated the diffusion process in enzyme–metal hybrid catalysts using Pd/lipase-Pluronic conjugates and the combination of immobilized lipase (Novozyme 435) and Pd/C as models. With reference to experimental data in previous studies, the Weisz–Prater parameter and efficiency factor of internal diffusion were calculated to evaluate the internal diffusion limitations in these catalysts. Thereafter, a kinetic model was developed and fitted to describe the proximity effect in hybrid catalysts. Results indicated that the enhanced catalytic efficiency of hybrid catalysts may arise from the decreased internal diffusion limitation, size effect of Pd clusters and proximity of the enzyme and metal active sites, which provides a theoretical foundation for the rational design of enzyme–metal hybrid catalysts.

关键词： enzyme–metal hybrid catalyst     internal diffusion     proximity effect     kinetic model    

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Microwave-assisted catalyst-free hydrolysis of fibrous cellulose for deriving sugars and biochemicals

Songshan Jiang, Helen Daly, Huan Xiang, Ying Yan, Huiping Zhang, Christopher Hardacre, Xiaolei Fan

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 718-726 doi: 10.1007/s11705-019-1804-5

摘要： Microwave (MW) assisted catalyst-free hydrolysis of fibrous cellulose (FC, cellulolysis) at 200°C promoted a cellulose conversion of ca 37.2% and quantitative production of valuable C5/C6 sugars (e.g , glucose) and the according platform biochemicals (e.g , 5-hydroxymethylfurfural), corresponding to an overall selectivity of 96.5%. Conversely, conventional hydrothermal cellulolysis under similar conditions was not effective, even after 24 h, carbonising the FC. Based on the systematic study of MW-assisted cellulolysis, the specific interaction between water molecules and macroscopic FC under the MW irradiation was proposed, accounting for the interpretation of the experimental observation. The kinetic energy of water molecules under the MW irradiation facilitated the C C (in the non-hindered surface CH OH groups) and C O C bond breaking (inside the cellulose cavities) in FC, producing primary cellulolysis products of xylose, glucose and cellobiose.

关键词： microwave     fibrous cellulose     hydrolysis     sugars     mechanism    

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Micro-sized hydrothermal carbon supporting metal oxide nanoparticles as efficient catalyst for mono-dehydration

Cheng PAN, Chao FAN, Wanqin WANG, Teng LONG, Benhua HUANG, Donghua ZHANG, Peigen SU, Aqun ZHENG, Yang SUN

《能源前沿（英文）》 2022年 第16卷 第5期   页码 822-839 doi: 10.1007/s11708-020-0677-0

摘要： Most known catalytic dehydration of sugar alcohols such as D-sorbitol and D-mannitol can only produce di-dehydrated forms as major product, but mono-dehydrated products are also useful chemicals. Moreover, both di- and mono-dehydration demand a high temperature (150°C or higher), which deserves further attentions. To improve the mono-dehydration efficiency, a series of metal-containing hydrothermal carbonaceous materials (HTC) are prepared as catalyst in this work. Characterization reveals that the composition of preparative solution has a key influence on the morphology of HTC. In transformation of D-sorbitol, all HTC catalysts show low conversions in water regardless of temperature, but much better outputs are obtained in ethanol, especially at a higher temperature. When D-mannitol is selected as substrate, moderate to high conversions are obtained in both water and ethanol. On the other hand, high mono-dehydration selectivity is obtained for both sugar alcohols by using all catalysts. The origin of mono-dehydration selectivity and role of carbon component in catalysis are discussed in association with calculations. This study provides an efficient, mild, eco-friendly, and cost-effective system for mono-dehydration of sugar alcohols, which means a lot to development in new detergents or other fine chemicals.

关键词： hydrothermal carbon     morphology     catalyst     mono-dehydration     sugar alcohol    

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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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Fischer-Tropsch synthesis by reduced graphene oxide nanosheets supported cobalt catalysts: Role of support and metalnanoparticle size on catalyst activity and products selectivity

Hasan Oliaei Torshizi, Ali Nakhaei Pour, Ali Mohammadi, Yahya Zamani, Seyed Mehdi Kamali Shahri

《化学科学与工程前沿（英文）》 2021年 第15卷 第2期   页码 299-309 doi: 10.1007/s11705-020-1925-x

摘要： In this paper, a series of cobalt catalysts supported on reduced graphene oxide (rGO) nanosheets with the loading of 5, 15 and 30 wt-% were provided by the impregnation method. The activity of the prepared catalysts is evaluated in the Fischer-Tropsch synthesis (FTS). The prepared catalysts were carefully characterized by nitrogen adsorption-desorption, hydrogen chemisorption, X-ray diffraction, Fourier transform infrared spectroscopy, Raman spectroscopy, temperature programmed reduction, transmission electron microscopy, and field emission scanning electron microscopy techniques to confirm that cobalt particles were greatly dispersed on the rGO nanosheets. The results showed that with increasing the cobalt loading on the rGO support, the carbon defects are increased and as a consequence, the reduction of cobalt is decreased. The FTS activity results showed that the cobalt-time yield and turnover frequency passed from a maximum for catalyst with the Co average particle size of 15 nm due to the synergetic effect of cobalt reducibility and particle size. The products selectivity results indicated that the methane selectivity decreases, whereas the C selectivity raises with the increasing of the cobalt particle size, which can be explained by chain propagation in the primary chain growth reactions.

关键词： cobalt catalyst     cobalt particle size     Fischer-Tropsch synthesis     reduced graphene oxide     supported catalyst    

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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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标题 作者 时间 类型 操作

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

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

期刊论文

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

Zhiyi Wu,Zafar Iqbal,Xianqin Wang

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

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

Tao Zhang, Tewodros Asefa

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

Rosin side chain type catalyst-free vitrimers with high cross-link density, mechanical strength, and

期刊论文

Exploration of the oxygen transport behavior in non-precious metal catalyst-based cathode catalyst layer

Shiqu CHEN, Silei XIANG, Zehao TAN, Huiyuan LI, Xiaohui YAN, Jiewei YIN, Shuiyun SHEN, Junliang ZHANG

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

Diffusion process in enzyme–metal hybrid catalysts

期刊论文

Microwave-assisted catalyst-free hydrolysis of fibrous cellulose for deriving sugars and biochemicals

Songshan Jiang, Helen Daly, Huan Xiang, Ying Yan, Huiping Zhang, Christopher Hardacre, Xiaolei Fan

期刊论文

Micro-sized hydrothermal carbon supporting metal oxide nanoparticles as efficient catalyst for mono-dehydration

Cheng PAN, Chao FAN, Wanqin WANG, Teng LONG, Benhua HUANG, Donghua ZHANG, Peigen SU, Aqun ZHENG, Yang SUN

期刊论文

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

Gang WU

期刊论文

Fischer-Tropsch synthesis by reduced graphene oxide nanosheets supported cobalt catalysts: Role of support and metalnanoparticle size on catalyst activity and products selectivity

Hasan Oliaei Torshizi, Ali Nakhaei Pour, Ali Mohammadi, Yahya Zamani, Seyed Mehdi Kamali Shahri

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