Article
Chemistry, Physical
Yingxin Feng, Xueting Wang, Ton V. W. Janssens, Peter N. R. Vennestrom, Jonas Jansson, Magnus Skoglundh, Henrik Gronbeck
Summary: The study shows that NH3-SCR on Cu-CHA is facilitated by NH3-solvated Cu sites, promoting the selective reduction of NO; NH3 adsorption inhibits the reaction at low temperatures; the successful formulation of a first-principles microkinetic model links kinetic behavior with materials properties.
Article
Engineering, Environmental
Kuo Liu, Hong He, Biwu Chu
Summary: A comprehensive microkinetic model was established for NO oxidation, standard SCR and fast SCR on CeWOx at low temperatures, revealing different rate-limiting steps and reaction orders for different reactions. The mechanisms of standard and fast SCR were found to be similar, with the reaction between nitrites and adsorbed NH3 playing a key role in NOx conversion. The activation energy of fast SCR was higher due to the reaction between NO and NH4NO3, but more nitrites and NH4NO3 led to higher activity for fast SCR compared to standard SCR.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Materials Science, Multidisciplinary
Yuta Kataoka, Jun Haruyama, Osamu Sugino
Summary: We calculated the diffusion coefficient of hydrogen on metal surfaces using a method that combines diagonalization of the potential energy surface with transition state theory. By including quantum effects and entropy effects in the transition state theory without stochastic simulations, our method provides more accurate results. However, more sophisticated quantum mechanical schemes are needed for cryogenic temperatures.
Article
Chemistry, Multidisciplinary
Kyungseok Lee, Byungchul Choi
Summary: A combined Ag/Al2O3 and Pd/Al2O3 catalyst was found to be effective for the selective catalytic reduction of NOx by H-2-assisted C3H6. The sequential arrangement of 1 wt% Ag/Al2O3 followed by 1Pd/Al2O3 enabled the reduction of NOx, C3H6, CO, and H-2 over wide reaction temperatures, with negligible formation of by-products.
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
(2021)
Article
Chemistry, Physical
Rohil Daya, Dylan Trandal, Unmesh Menon, Dhruba J. Deka, William P. Partridge, Saurabh Y. Joshi
Summary: In this study, a kinetic model is developed for the reduction and oxidation reactions of Cu sites in Cu-SSZ-13. The rate parameters of these reactions are investigated using Fourier transform infrared spectroscopy and spatially resolved mass spectrometry. The model is validated with experimental measurements and successfully predicts the formation and consumption of nitrogen oxides. NH3 release is observed during the oxidation reaction at low temperatures, and the presence of NH3 negatively affects the catalyst's activity. This study provides important insights into the reduction and oxidation mechanisms of Cu-SSZ-13 catalysts.
Article
Chemistry, Physical
Wenbo Xie, Jiayan Xu, Yunxuan Ding, P. Hu
Summary: Selective acetylene hydrogenation on Pd(111) was comprehensively investigated using a detailed microkinetic model developed with density functional theory energies. By combining coverage-dependent calculations and AIMD results, a full first-principles kinetic simulation was achieved, showing that the coverage-dependent model gives more reasonable results. The study found that the activity is mainly influenced by the barriers of the first two hydrogenation steps, with ethylene desorption and C2H4* hydrogenation barriers significantly impacting selectivity, particularly the former.
Article
Chemistry, Multidisciplinary
Shiyu Xu, Yiyang Zhang, Christopher Hardacre, Zhiming Liu
Summary: The Pd/TiO2 nanowire catalyst exhibited higher H-2-SCR activity and wider activity temperature range compared to the Pd/TiO2 nanoparticle catalyst. This is attributed to the larger surface area, higher Pd dispersion, higher metallic Pd content, and increased surface adsorbed oxygen of the nanowire structure, which enhance the adsorption and activation of NO x and the spillover of hydrogen.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Energy & Fuels
Guozhen Qin, Yining Zhang, Jianfeng Zheng, Yifan Li, Xiaojin Han, Zhanggen Huang
Summary: Iron-based catalysts show great potential for selective catalytic reduction of NOx with NH3 (NH3-SCR) due to their excellent SCR activity, N2 selectivity, and environmental performance. In this study, the reaction pathway of NH3-SCR on the Fe3O4(111) surface was investigated using density functional theory (DFT) and experimental measurements. The research findings revealed that the surface favored the adsorption of NO molecules and followed the NO activation mechanism.
Article
Chemistry, Physical
Hai-Yan Su, Wenbo Liao, Keju Sun
Summary: Molybdenum disulfide (MoS2) is a promising non-precious metal catalyst for CO2 hydrogenation, but the exact reaction mechanism and active site are still debated. This study investigates the competitive pathways for CO, methane, and methanol formation on the S edge site of MoS2 catalyst using DFT calculations and microkinetic modeling. It reveals that CO is exclusively produced through a redox mechanism on the S edge, with Mo edge as the likely active site. This work provides a mechanistic understanding of CO2 hydrogenation on MoS2 catalyst, and can aid in designing improved catalysts for important technological reactions.
APPLIED SURFACE SCIENCE
(2023)
Article
Chemistry, Applied
Yingxin Feng, Derek Creaser, Henrik Gronbeck
Summary: This study presents a first-principles based kinetic model to analyze the reaction steps that control the selectivity and light-off temperature in NH3-SCR. A simplified kinetic model is developed for accurate description of the reaction. The findings provide insight into the design of efficient Cu-CHA catalysts.
TOPICS IN CATALYSIS
(2023)
Article
Chemistry, Physical
Raquel J. Rama, Celia Maya, Francisco Molina, Ainara Nova, M. Carmen Nicasio
Summary: 2-Aminobiphenyl palladacycles are successful precatalysts for Pd-catalyzed cross-coupling reactions. This study investigates the mechanism of aryl amination reactions catalyzed by a cationic 2-aminobiphenyl palladacycle supported by a terphenyl phosphine ligand. The results show that the formation of an aryl carbazolyl Pd(II) complex reduces catalyst decomposition and can be considered as an alternative precatalyst in cross-coupling reactions.
Article
Chemistry, Physical
Qingbo Wang, Jiaqiang Yang, Zhang Liu, Yanwei Wen, Rong Chen, Bin Shan
Summary: In this study, the NO oxidation properties of pristine and 3d transition metal doped ZnMn2O4 were investigated using first principles calculations and microkinetic analysis. It was found that there are two different mechanisms of NO oxidation on different catalysts, with Cu and Fe doping showing the best low-temperature NO oxidation performance.
APPLIED SURFACE SCIENCE
(2022)
Article
Nanoscience & Nanotechnology
Shiyu Xu, Ruoyuan Li, Jianjun Chen, Zhiming Liu
Summary: A high-activity Pd supported on TiO2 coating on a SiO2 nanosphere catalyst has been developed for selective catalytic reduction of NO x by H-2 (H-2-SCR). The coating structure of TiO2 on the SiO2 nanosphere plays a crucial role in the catalyst's performance. Compared to Pd supported on TiO2 particles, the Pd/SiO2-TiO2(C) catalyst exhibits higher activity, smaller Pd particle size, more surface chemisorbed oxygen, and metallic Pd species, resulting in improved performance.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Applied
Yiyang Zhang, Hui Zeng, Bin Jia, Zhiming Liu
Summary: The Pd/FeTi catalyst showed higher H-2-SCR activity compared to Pd/Ti and Pd/Fe catalysts, mainly due to the formation of FeTi solid solution and highly dispersed Pd on the support.
Article
Nanoscience & Nanotechnology
Zhang Liu, Jiaqiang Yang, Yanwei Wen, Yuxiao Lan, Limin Guo, Xi Chen, Kun Cao, Rong Chen, Bin Shan
Summary: This study investigates the mechanism of CO PROX reaction on Co3O4 supported single Pt atom through first-principles based microkinetic analysis. The research finds that H2 prereduction treatment effectively mitigates the CO poisoning effect and surface H atoms assist in improving the activity and selectivity at low temperatures.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Chen Zhu, Jing-Pei Cao, Zhen Yang, Xiao-Yan Zhao, Wen-Cai Yi, Xiao-Bo Feng, Yun-Peng Zhao, Hong-Cun Bai
Summary: By using computational techniques, the hydrodeoxygenation mechanism of anisole on Ni surface was investigated. The results showed that phenol was the major product on clean Ni surface, while methylcyclohexane was the main product on H-covered Ni surface. These findings provide mechanistic understanding for the conversion of anisole under different experimental conditions.
MOLECULAR CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Jingbin Li, Wencai Yi, Meng Yin, Haifeng Yang, Junfang Li, Yahui Li, Zhiwei Jiao, Hua Bai, Mingqiang Zou, Guangcheng Xi
Summary: In this study, ultrathin multilayer rhenium (Re) nanosheets were found to exhibit extraordinary surface enhanced Raman scattering (SERS) performance as a rare-earth metal substrate. These Re nanosheets, prepared through a low-temperature molten salt strategy, showed high sensitivity, chemical stability, and signal repeatability. The composite enhancement mechanism caused by localized surface plasmon resonance (SPR) and charge transport played an important role in the rare-earth-SERS system. Furthermore, the Re nanosheets were capable of high-throughput multiassay analysis, allowing rapid separation and identification of various analytes.
Article
Chemistry, Physical
Xingang Jiang, Tao Yang, Ge Fei, Wencai Yi, Xiaobing Liu
Summary: Researchers have reported a new type of two-dimensional graphene material with good stability and high Fermi velocities. Some of the monolayers exhibit a pristine n-type self-doping Dirac cone structure, while the ClPSi3 monolayer is found to be potential excellent strain sensor.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Xinyong Cai, Wencai Yi, Jiao Chen, Linguo Lu, Bai Sun, Yuxiang Ni, Simon A. T. Redfern, Hongyan Wang, Zhongfang Chen, Yuanzheng Chen
Summary: By using structure design and simulation, researchers have discovered a new carbon nitride framework with high porosity and N content, which exhibits extremely high theoretical capacity and feasibility for experimental realization in lithium-ion batteries. Furthermore, the study found that this carbon nitride framework can be further expanded and constructed to maintain high Li storage capacity.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
Article
Nanoscience & Nanotechnology
Xingang Jiang, Guanghui Zhang, Wencai Yi, Tao Yang, Xiaobing Liu
Summary: This study demonstrates that the penta-BeP2 monolayer is an excellent sensor for toxic gases, showing high selectivity, sensitivity, and reversibility.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Damin Liu, Wencai Yi, Yanling Fu, Qinghong Kong, Guangcheng Xi
Summary: This study presents a mild and general in situ surface restraint-induced growth method for the preparation of highly crystalline tungsten nitride nanocrystals with excellent dispersibility, forming a hybrid structure in ultrathin carbon layers. These hybrid nanobelts exhibit strong localized surface plasmon resonance and surface-enhanced Raman scattering effects, with outstanding corrosion resistance, radiation resistance, and oxidation resistance, maintaining SERS performance in harsh environments. The synergistic Raman enhancement mechanism of LSPR and interface charge transfer is found in the carbon coated tungsten nitride substrate, enabling high-throughput dynamic SERS analysis in a microfluidic SERS channel.
Article
Chemistry, Analytical
Jingbin Li, Junfang Li, Wencai Yi, Meng Yin, Yanling Fu, Guangcheng Xi
Summary: This paper reports the surface-enhanced Raman spectroscopy performance of metallic niobium nitride three-dimensional hierarchical network structures. The unique nanocavity structure promotes the entry of molecules and takes advantage of electromagnetic hot spots, and the substrate exhibits outstanding environmental durability, high signal reproducibility, and detection universality.
ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Lu Zhang, Junfang Li, Wencai Yi, Guoying Wei, Meng Yin, Guangcheng Xi
Summary: Controlling the structure of graphdiyne (GDY) is important for exploring new properties and applications. This study presents the microemulsion synthesis of GDY hollow spheres and multiwalled nanotubes composed of ultrathin nanosheets for the first time. The formation of an oil-in-water microemulsion is found to be the key factor in controlling GDY growth. The resulting GDY hollow spheres have fully exposed surfaces, exhibiting an ultrahigh specific surface area of 1246 m2 g-1 and potential applications in water purification and Raman sensing.
Article
Physics, Multidisciplinary
Yuanyuan Wang, Zhihui Li, Shifeng Niu, Wencai Yi, Shuang Liu, Zhen Yao, Bingbing Liu
Summary: In this study, Ce-N compounds were systematically explored using first-principles calculations. It was found that the cerium atom can weaken the strength of the N=N bond and various cerium polynitrides can be formed under moderate pressure. Among them, P1-CeN6 has the lowest synthesis pressure (32 GPa) and exhibits high hardness and large volumetric energy density, indicating good structural stability and high energy density characteristics.
MATTER AND RADIATION AT EXTREMES
(2023)
Article
Nanoscience & Nanotechnology
Haiying Du, Zhaorui Zhang, Xingang Jiang, Jing Wang, Wencai Yi, Xiaogan Li, Jinkui Chu
Summary: A new technique of polarization doping was used to improve the NO2 gas sensing performance of the polypyrrole sensor. The introduction of sodium dodecyl benzenesulfonate enhanced the dispersion and specific surface area of the PPy nanosheets. The resulting PPy sensor showed excellent NO2 sensing properties due to the enhanced adsorption ability and electron transfer caused by polarization doping.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Multidisciplinary Sciences
Lu Zhang, Wencai Yi, Junfang Li, Guoying Wei, Guangcheng Xi, Lanqun Mao
Summary: In this study, a surfactant-free growth method was developed to efficiently synthesize graphdiyne hollow microspheres with a self-supporting structure. Pristine graphdiyne hollow microspheres were found to exhibit a strong surface-enhanced Raman scattering effect without any additional functionalization, which can be attributed to efficient interfacial charge transfer within the graphdiyne-molecule system.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Shuai Han, Yunxian Liu, Chao Wang, Wencai Yi, Xin Chen, Yongsheng Zhang, Xiaobing Liu
Summary: Elemental boron has attracted considerable interest due to its electron deficiency, which allows for the formation of multicenter bonds and various stable and metastable allotropes. Through first-principles calculations and structure search, boron-rich K-B binary compounds have been investigated, leading to the prediction of dynamically stable structures containing boron framework with open channels. Furthermore, four novel boron allotropes were discovered to possess dynamical, thermal, and mechanical stability at ambient pressure, with o-B-14 exhibiting an unusual bonding combination and potential superconductivity.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Wenjuan Li, Yipin Zhang, Yuhua Wang, Weiguang Ran, Qinhui Guan, Wencai Yi, Lulu Zhang, Dapeng Zhang, Na Li, Tingjiang Yan
Summary: In this study, graphdiyne (GDY) was introduced for the first time into the gaseous photocatalytic CO2 hydrogenation system, and a GDY-modified In2O3 nanocomposite (GDY-IO) was fabricated. GDY-IO showed improved performance in CO2 hydrogenation, resulting in higher yields of C1 (CO and CH4) and formation of C2+ hydrocarbons (C2H4, C2H6, C3H6, and C3H8). The introduction of GDY promoted electron transport and suppressed carrier recombination, leading to enhanced CO2 hydrogenation reaction. The GDY-IO interface stabilized key intermediates and reduced the kinetics barrier, facilitating thermodynamically favorable exothermal processes. This research opens up a new avenue for the synthesis of high value-added chemical fuels from greenhouse gases.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2024)
Article
Materials Science, Multidisciplinary
Taowen Dong, Wencai Yi, Ting Deng, Tingting Qin, Xianyu Chu, He Yang, Lirong Zheng, Seung Jo Yoo, Jin-Gyu Kim, Zizhun Wang, Yan Wang, Wei Zhang, Weitao Zheng
Summary: This study investigates the conversion reaction mechanism of α-Fe2O3 and reveals the impact of diffusional and diffusionless transformation on electrochemical performance, as well as a method to achieve pseudocapacitance through diffusionless transformation.
ENERGY & ENVIRONMENTAL MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Lei Zhao, Shijie Liu, Yuanzheng Chen, Wencai Yi, Darlar Khodagholian, Fenglong Gu, Eric Kelson, Yonghao Zheng, Bingbing Liu, Mao-sheng Miao
Summary: All-nitrogen solids have great potential as high-energy-density materials, but currently can only be obtained through high-pressure synthesis. Molecular crystals, compared to covalent solids, have higher stability during decompression. This study demonstrates that the design of a novel N-16 molecule and its crystal structure can lead to the formation of an all-nitrogen molecular crystal with favorable properties.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Physical
Yifan Sun, Ye Lv, Wei Li, Jinli Zhang, Yan Fu
Summary: In this study, PtRu electrocatalysts were fabricated on carbon paper via cyclic electrodeposition for the electrocatalytic hydrogenation (ECH) of phenol. The Pt3Ru3 catalyst exhibited excellent activity and stability for the conversion of phenol to cyclohexanol at ambient temperature and various current densities. The in situ Raman spectroscopy and kinetic study revealed the hydrogenation mechanism of phenol over Pt3Ru3 in acidic electrolyte, providing an effective electrochemical strategy for the facile construction of durable electrode materials and efficient phenol hydrogenation.
JOURNAL OF CATALYSIS
(2024)
Article
Chemistry, Physical
Amir Shahzad, Khezina Rafiq, Muhammad Zeeshan Abid, Naseem Ahmad Khan, Syed Shoaib Ahmad Shah, Raed H. Althomali, Abdul Rauf, Ejaz Hussain
Summary: Photocatalytic hydrogen production through water splitting is an effective method for meeting future energy demands. In this study, researchers synthesized a 1 % Ag2S/Cu2S co-doped CdZnS catalyst and found that it can produce hydrogen at a higher rate. The co-doping of Ag2S and Cu2S in the CdZnS catalyst showed a synergistic effect, with Ag2S promoting oxidation reactions and Cu2S promoting reduction reactions.
JOURNAL OF CATALYSIS
(2024)