Review
Chemistry, Physical
Zhuohua Sun, Zhe-Hui Zhang, Tong-Qi Yuan, Xiaohong Ren, Zeming Rong
Summary: This review explores the history, synthetic strategies, and controls of Raney Ni catalysts, with a focus on their applications in biomass conversion. By comparing with supported Ni catalysts, the unique advantages of Raney Ni in biomass conversion are revealed.
Article
Chemistry, Multidisciplinary
Bogdan Shumeiko, David Kubicka
Summary: Lignin can be converted into useful precursors of fuels and fine chemicals through mild hydrogenation, which is affected by the complexity of the reactant and the position of the functional group. Different solvents also have an impact on the conversion of phenols.
Article
Engineering, Chemical
Haoan Fan, Bolong Li, Xuezhi Zhao, Zhecheng Fang, Chao Chen, Wenhua Zhou, Wulong Yang, Mian Li, Xiuyang Lu, Jie Fu
Summary: The kinetics and mechanisms of selective maltose hydrogenation over Raney Ni were investigated in this study. Optimization of reaction conditions illustrated that maltitol formation was favored by moderate reaction temperatures, high hydrogen pressures, and near-neutral sodium phosphate buffer. The kinetic studies showed an activation energy of 45.5 kJ/mol for the hydrogenation of maltose. In situ IR and UV-vis spectra provided insights into the mechanism of the hydrogenation process. This study contributes to the industrial development of maltitol manufacturing.
Article
Engineering, Chemical
Xin Zhang, Wei-Kun Jiang, Bao-Ju Wang, Xiang-Yang Cui, Zhi-Yong Tang, Hai-Kui Zou, Guang-Wen Chu, Yong Luo
Summary: The intrinsic kinetics of catalytic hydrogenation of p-nitroanisole (PNA) to p-aminoanisole have been investigated in this study. Experimental and theoretical analyses were conducted under different conditions to determine the kinetic characteristics. Power law analysis revealed reaction orders for hydrogen and PNA, and Eley-Rideal and Langmuir-Hinshelwood-Hougen-Watson (LHHW) models were used to fit the data. The adsorption of dual-site dissociative H2 was identified as the rate-controlling step based on the LHHW model.
CHEMICAL ENGINEERING RESEARCH & DESIGN
(2022)
Article
Engineering, Environmental
Lei Zuo, Junfeng Wang, Deqing Mei, Derick Adu-Mensah, Yaping Gao
Summary: The study investigated the ultrasonic-assisted CTH process for biodiesel, which effectively controlled the generation of C18:0 and trans-C18:1. The optimum reaction conditions were found to be reaction temperature of 80°C, stirring rate of 600 rpm, catalyst dosage of 10 wt%, isopropanol amount of 32 g, and water amount of 100 g. The ultrasonic field reduced the selectivity of trans-C18:1 and decreased the iodine value of biodiesel.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Engineering, Chemical
Shutao Wu, Hongliang Zhang, Xun Huang, Qiang Liao, Zidong Wei
Summary: The electrochemical dimerization of acrylonitrile on metal cathodes is a simple and green method for producing adiponitrile, the raw material for nylon 66. The production rate of ADN and byproducts is highly related to the surface adsorption state, where high ADN selectivity is obtained when the surface is mainly covered by AN. Substitution of AN with hydrogen promotes surface hydrogenation to form propionitrile, while a full coverage of hydrogen exclusively leads to hydrogen evolution.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Article
Chemistry, Multidisciplinary
Ruth D. Mojica Sepulveda, Luis J. Mendoza Herrera, Delia B. Soria, Virginia Vetere, Eduardo E. Grumel, Carmen I. Cabello, Marcelo Trivi, Myrian C. Tebaldi
Summary: We investigated the influence of various physical-chemical parameters on the selective reaction of acetophenone hydrogenation using different nickel catalysts on clinoptilolite supports. The aim of this study is to identify the combination of parameters that allows for obtaining the best catalytic results.
Article
Chemistry, Multidisciplinary
Jianglong Pu, Changhao Liu, Shenming Shi, Junxian Yun
Summary: In this study, porous Al2O3-encapsulated RANEY (R) nickel and alumina-supported Ni-Ru bimetallic catalysts were designed and synthesized to improve the activity and stability in the hydrogenation of MTHPA to MHHPA. The encapsulation of porous Al2O3 enhanced the stability of the Ni skeleton and adsorption ability of the reactant molecules, while the introduction of Ru improved the dispersion and stability of metallic Ni. However, it also increased the hydrogenation difficulties.
Article
Chemistry, Physical
Zhecheng Fang, Haoan Fan, Xuezhi Zhao, Gaobo Lin, Bolong Li, Jianghao Wang, Xiuyang Lu, Wulong Yang, Mian Li, Weiyu Song, Jie Fu
Summary: This study reveals the nature of glucose hydrogenation on Raney Ni catalysts, and provides directions for the design of highly efficient nickel-based catalysts.
APPLIED CATALYSIS A-GENERAL
(2023)
Article
Chemistry, Physical
Brett Pomeroy, Miha Grilc, Saso Gyergyek, Blaz Likozar
Summary: This study presents a novel experimental and theoretical investigation of hydroxymethylfurfural hydrogenation using ceria-doped Ni/Al2O3 catalysts with and without water-containing media. It was found that the ceria-doped catalyst showed improved reducibility but lower reaction rates and TOFs compared to the unpromoted catalyst. However, the NiCe/Al2O3 catalyst exhibited enhanced ring opening and ring-saturation capability due to modifications of surface sites. The addition of water as a co-solvent eliminated deoxygenation reactions and resulted in specific products.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Achraf Sadier, Dichao Shi, Anne-Sophie Mamede, Sebastien Paul, Eric Marceau, Robert Wojcieszak
Summary: The bimetallic Ni-Fe catalyst showed better activity and stability in the aqueous phase hydrogenation of xylose compared to the monometallic Ni catalyst. A temperature of 80 degrees Celsius was found to minimize nickel leaching.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Engineering, Chemical
Chong Peng, Peng Liu, Zhiming Zhou, Xiangchen Fang, Yun-Xiang Pan
Summary: In this study, detailed thermodynamic and kinetic analyses were performed on the hydrogenation of phenanthrene using a Ni-Mo/HY catalyst. A comprehensive reaction network was established and a kinetic model with 28 parameters was constructed. The most favorable pathway for the hydrogenation of phenanthrene was identified. These findings provide guidance for optimizing catalyst properties and reaction conditions for phenanthrene hydrogenation.
Article
Chemistry, Multidisciplinary
Xiaohong Ren, Zhuohua Sun, Jiqing Lu, Jinling Cheng, Panwang Zhou, Xiaoqiang Yu, Zeming Rong, Changzhi Li
Summary: In this study, a novel method for upgrading biomass-derived phenolic monomers through hydrogen-free hydrodeoxygenation (HDO) was proposed and evaluated. The HDO process was combined with the activation of water and aqueous phase reforming of in situ generated methanol over a nano-porous Ni catalyst, resulting in a one-pot approach with high selectivity of bio-phenol. DFT calculations confirmed the crucial role of the Ni catalyst in activating water and facilitating the subsequent HDO process.
Article
Engineering, Chemical
Xiang Yang Cui, Xin Zhang, Baoju Wang, Yu-Qi Sun, Hai Kui Zou, Guang Wen Chu, Yong Luo, Jian Feng Chen
Summary: In this study, the kinetic models of NMA hydrogenation to AMA catalyzed by Raney nickel catalyst were investigated. The reaction was found to follow 0.52-order kinetics with respect to the NMA concentration and 1.10-order kinetics in terms of hydrogen pressure. Based on the LHHW model, the dual-site dissociation adsorption of hydrogen was identified as the rate determining step.
CHINESE JOURNAL OF CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Jianli Chen, Feng Xu, Fengqiang Ma, Minna Ren, Jiadi Zhou, Zhiqun Yu, Weike Su
Summary: The method of combining TPP with Raney Ni in continuous flow is proposed to improve the chemical selectivity of anilines prepared by nitroarenes hydrogenation. Analysis of ICP, FT-IR, XRD, and EDS suggests that low degree of complexation and uniform distribution of TPP play key roles. TPP/Raney Ni exhibits excellent tolerance to halogens and unsaturated functional groups, and the practicality of the continuous flow system has been tested.
JOURNAL OF FLOW CHEMISTRY
(2021)
Article
Chemistry, Physical
Xing Liu, Yunpeng Hou, Fangqi Yang, Yueyue Liu, Haoming Yu, Xinxin Han, Jingwen Chen, Shixia Chen, Shaodong Zhou, Shuguang Deng, Jun Wang
Summary: In this study, novel electrocatalysts Ni@NCNT were synthesized by encapsulating Ni nanoparticles in N-rich carbon nanotubes using chemical vapor deposition method. The optimized Ni@NCNT-700 showed high Faradic efficiency for ethanol synthesis in a wide potential range, with ethanol as the sole liquid product. In-situ Raman and density functional theory calculations revealed that the synergistic effects of Ni nanoparticles and NCNTs lowered the energy barrier for C-C coupling and suppressed *CO desorption.
Article
Chemistry, Physical
Bowei Yuan, Shi-Ya Tang, Shaodong Zhou
Summary: This paper reviews the fundamental aspects of the challenges related to C-H activation in gas-phase cluster reactions. The size effect is found to play a crucial role in regulating both the reactivity and selectivity of the activation processes. The authors discuss the size effect in hydrocarbon oxidation by early transition metal oxides and main group metal oxides, as well as in methane activation mediated by late transition metals, based on mass-spectrometry experiments and quantum chemical calculations.
Article
Chemistry, Multidisciplinary
Xi He, Weili Song, Xuemin Liu, Jiamin Huang, Ruilong Feng, Shaodong Zhou, Jianquan Hong, Xin Ge
Summary: A sustainable and general multicomponent cross-coupling method for the synthesis of 3-chalcogenylindoles from indoles using aryl iodides and elemental sulfur under aqueous micellar conditions is developed. Elemental sulfur serves as an eco-friendly and easy-handling sulfur source, generating thiyl radicals. The synergic effect between Cu catalysts and micelles formed by the sugar-based surfactant GluM stabilizes thiyl radicals, enabling C-S coupling with readily available indoles through single-electron transfer. The aqueous micellar system can be recycled and reused with good yields and can also be extended to the conversion of elemental selenium.
Article
Chemistry, Physical
Shihan Li, Xiao-Nan Wu, Shaodong Zhou
Summary: Gas-phase reactions of [OsC3](+) with methane at ambient temperature were studied using quadrupole-ion trap mass spectrometry combined with quantum chemical calculations. Comparison with product clusters revealed significant changes in cluster reactivity. Theoretical calculations showed that electronic features such as molecular polarity index, charge and spin distribution, and HOMO-LUMO gap had an influence on the reactivity of the Os complexes. The polarity of the clusters played a fundamental role in the methane activation. Lowering the local polarity of the catalyst active site may reduce the formation of byproducts in the reaction.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Mengdi Guo, Shaodong Zhou, Xiaoyan Sun
Summary: Inspired by nature, the oxidation process of methane by the high-valent iron oxide cation [FeO2]+ was studied using FT-ICR mass spectrometry and quantum chemical calculations. Unlike previous systems, the reaction of [FeO2]+ with CH4 primarily generates Fe+ instead of [FeOH]+. Theoretical calculations suggest a novel oxygen rebound pathway for the liberation of methanediol. This study bridges the gap between gas-phase models and condensed-phase biosystems.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Agronomy
Xin Wang, Shaodong Zhou, Jie Wang, Wenxin Lin, Xiaolei Yao, Jiaqing Su, Haiyang Li, Chao Fang, Fanjiang Kong, Yuefeng Guan
Summary: This study investigated the genetic basis of biomass accumulation in soybean plants. It identified 10 loci and 47 candidate genes related to biomass traits, and highlighted a potential candidate gene for future soybean breeding.
MOLECULAR BREEDING
(2023)
Article
Engineering, Chemical
Xinpei Wang, Chao Qian, Shi-Ya Tang, Shaodong Zhou
Summary: This study couples ammonia synthesis with methane conversion under plasma conditions using Fe-Al composite metal oxides as catalyst, resulting in shortened process for ammonia production and high selectivity in generating C-2 hydrocarbon byproducts. To overcome the activation barrier for methane and nitrogen, dielectric barrier discharge technology is employed to input high-quality energy into the reaction system. Examination of various 3d-metal oxides, SiO2, and Al2O3 leads to the identification of Fe-Al composite metal oxide as the catalyst of choice. The catalyst's structure is characterized using XRD, XPS, TGA, and BET techniques.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Inorganic & Nuclear
Jin Lv, Mincheng Yu, Jie Qin, Shaodong Zhou
Summary: This study investigates the liquid-phase activation of methane by ruthenium complexes using experiments and quantum-chemical calculations. It is surprising that methane can be efficiently converted to methyl trifluoroacetate under mild conditions, with the bis(NHC) ligand performing better than the other ligands. The study discusses the electronic origins of the exceptional performance of the ruthenium complex, focusing on ligand effects, and identifies the dative C & RARR; Ru interaction and structural distortion of the bis(NHC) plane as responsible factors. This work highlights the promising role of ruthenium in the development of efficient organometallic catalysts for methane conversion.
INORGANICA CHIMICA ACTA
(2023)
Article
Chemistry, Physical
Shihan Li, Chao Qian, Xiao-Nan Wu, Shaodong Zhou
Summary: Gas-phase reactions of [MC]+ (M = Os and Ru) with methane at ambient temperature have been studied by using quadrupole-ion trap (Q-IT) mass spectrometry combined with quantum chemical calculations. Theoretical calculations reveal the influence of electronic signatures and that it is the energy gap of the associated frontier molecular orbitals that dominates the ability of the cluster in the initial H3C-H bond breaking. Additionally, factors like the dipole moment, spin density, and charge distributions influence the orbital energy gap to different extents, suggesting that altering the local structure of the active center could regulate the activity.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Zihan Lv, Zeng Hong, Chao Qian, Shaodong Zhou
Summary: Pt-Pd alloy nano-catalysts supported on TiO2 were developed for efficient light-induced photocatalytic N-alkylation of amines with alcohols. Various techniques were utilized to characterize the catalysts and the photocatalytic mechanism was discussed. Pt served as a hydrogen shuttle, extracting hydrogen from alcohols to Pd for subsequent hydrogenation. By adjusting the Pd/Pt ratio, the reaction rates of methanol dehydrogenation and imine hydrogenation could be tuned simultaneously, leading to an efficient N-alkylation reaction. The Pd1Pt1/TiO2 catalyst exhibited excellent catalytic performance surpassing previous reports in terms of both efficiency and capacity.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Review
Chemistry, Multidisciplinary
Shuyue Wang, Chao Qian, Shaodong Zhou
Summary: The discovery of the Haber-Bosch process played a significant role in the industrial synthesis of ammonia in the early 20th century, contributing to the evolution of human society. Currently, the electrocatalytic reduction of nitrogen (NRR) offers a promising alternative technology for ammonia production under mild conditions, being a clean process without noticeable environmental impact. However, the challenge lies in achieving the desired reaction rate and efficiency due to the difficulty in breaking N = N bonds.
MATERIALS CHEMISTRY FRONTIERS
(2023)
Article
Multidisciplinary Sciences
Jinming Fan, Chao Qian, Shaodong Zhou
Summary: This paper presents a corrected group contribution (CGC)-molecule contribution (MC)-Bayesian neural network (BNN) protocol for accurate prediction of absorption spectra. By combining BNN with CGC methods, accurate and efficient prediction of full absorption spectra of various molecules is achieved using a small dataset for training.
Article
Chemistry, Physical
Yanyan Liu, Shuyue Wang, Minghao Sun, Min Ling, Shaodong Zhou, Chengdu Liang
Summary: This study reports a method of inducing homogeneous lithium deposition by minimizing the surface energy discrepancy of lithium crystal faces, successfully achieving dendrite-free lithium anode and exhibiting excellent electrochemical performance in symmetric cells and full cells.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Lanxiang Yang, Shuyue Wang, Chao Qian, Shaodong Zhou
Summary: The synthesis and high performance of VS4-140 material in electrocatalytic nitrogen reduction are reported. First-principles calculations reveal the different behaviors of VS2 and VS4-140 in terms of reaction mechanism and electronic origins.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Jiapeng Ji, Yunpeng Hou, Shiyu Zhou, Tong Qiu, Liang Zhang, Lu Ma, Chao Qian, Shaodong Zhou, Chengdu Liang, Min Ling
Summary: This study investigates the oxygen evolution reaction (OER) activity of single-atom catalysts (SACs) and reveals that oxygen-coordinated atomic metal species exhibit unique catalytic properties due to the weaker M-O bond compared to the M-N bond. A series of metal-oxygen-carbon structured low-nucleus clusters (LNCs) were successfully anchored on the surface of multiwalled carbon nanotubes (M-MWCNTs) using a low-temperature gas transfer method. The synthesized Ni-MWCNTs electrocatalyst demonstrates excellent OER activity and stability under alkaline conditions, surpassing the performances of Co-MWCNTs, Fe-MWCNTs, and RuO2. Density functional theory calculations reveal that the oxidation of low-nucleus Ni clusters lowers the energy barrier of the OER rate-limiting step, making the OER process more energy-efficient. This study presents a novel versatile platform for large-scale manufacturing of oxygen-coordinated LNC catalysts.
