CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Haowei Liu,Tao Zheng,Tianli Hui,Rui Zhang,Xianghai Meng,Wenshuai Zhu,Haiyan Liu,Zhichang Liu
Conversion of ethanol to high-value alcohols is an attractive approach for developing renewable biofuels, the key is to develop stable and high-efficient catalysts. In this work, based on the preparation strategy of heteroatomic Beta zeolites, a bifunctional Pt-Y/Beta catalyst was prepared by solid-state ion exchange and impregnation. Through characterization techniques such as TEM, NMR and XAS, it was confirmed that the Y species were incorporated into the framework of Beta zeolite by interacting with the silanol groups located at the defect sites, while the Pt species were confirmed to be present on the surface of the zeolite in the form of dispersed nanoparticles . The unique structure form and the favorable spatial proximity of the two metallic active sites lead to a synergistic catalysis, which enable a one-step conversion of ethanol to n-butanol with exceptionally high selectivity of 68 %. In situ DRIFT characterization, ethanol-TPD and relay experiment results show that in the ethanol to n-butanol reaction, the Pt species in Pt-Y/Beta catalyst serves as the active center for the dehydrogenation of ethanol and the hydrogenation of crotonaldehyde and crotyl alcohol, while the Y species is responsible for catalyzing the condensation reaction of acetaldehyde.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Xingchi Li,Huaming You,Cheng Wang,Dongmei Liu,Rui Yu,Siyu Guo,Yuan Wang,Yukou Du
Modifying the electronic structure and optimizing the geometric structure can expeditiously tune the electrocatalytic properties of catalysts, resulting in considerably enhanced electrocatalytic performance towards electrocatalytic oxidation of liquid fuels . We herein report a simple synthetic strategy to prepare Bi-doped 3D taraxacum-like Pd nanocages (NCs) composed of porous nanosheets , which possess high surface areas and strong synergistic effects. Notably, a trace of Bi diffuses into the lattice of Pd and increases the electronic effects of the surface of Pd, endowing PdBi-0.5 NCs/C with superior electrocatalytic performance towards ethanol oxidation reaction (EOR). The mass activity and specific activity of PdBi-0.5 NCs/C were 3494.8 mA mg Pd −1 and 10.37 mA cm −2 , being 4.08- and 4.82- fold enhancements as compared with commercial Pd/C, respectively. Moreover, the highly open porous 3D nanocages structure with rich active sites and defects can also facilitate the mass/electron transfer to favor the EOR kinetics.
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Processes
·
2021
·Vol. 9
·期 2
·230
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IF 2.847
Peng Peng,Jun Li,Shengpeng Mo,Qi Zhang,Taiming Shen,Qinglin Xie
Carbon monoxide (CO) and hydrocarbons (HCs) generally have competitive adsorption on the active site of noble-metal nano-catalysts, thus developing an effective way to reduce the passivation of competitive reaction with each other is an urgent problem. In this study, we successfully synthesized transition metal-noble metal (Pt-M) alloys via introducing inexpensive metal elements (M = Ni, Co and Cu) into Pt particles and then deposited on alumina support to form Pt-based catalysts. Subsequently, we choose CO and toluene as polluting gases to evaluate the catalytic activities of Pt-M/Al2O3catalysts. Introducing inexpensive metal elements (M = Ni, Co, and Cu) significantly changed the physicochemical properties and catalytic activities of these Pt-based catalysts. It can be found that the Pt-Co/Al2O3catalyst exhibited outstanding catalytic activity for CO and toluene oxidation under mixed gas atmosphere, compared with other Pt-based catalysts, which is due to the higher dispersity, more surface adsorption oxygen, and well redox ability. Surprisingly, H2O could promote the catalytic activities for CO/toluene co-oxidation over the Pt-Co/Al2O3catalyst. Thus, the present synthetic strategy not only opens an avenue towards the synthesis of noble metal-based catalysts, but also provides an excellent tolerance to H2O in the catalytic process.Keywords:bimetallic alloy;Pt-based catalysts;catalytic oxidation;toluene;moisture
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Ying Deng,Zhenyu Xiao,Zuochao Wang,Jianping Lai,Xiaobin Liu,Dan Zhang,Yi Han,Shaoxiang Li,Wei Sun,Lei Wang
Following the guidance of nitrogenase, the natural iron-based catalysts with remarkably high activity in nitrogen reduction reaction (NRR) may be a talent option to develop artificial molecular mimics. However, the electrochemical NRR process of iron-based catalysts still suffers from the high overpotential, poor lifespan, and slow reaction kinetics of the hydrogenation process. Through a controllable etching and in-situ carbonating process, a Pt-doped FeP/C hollow nanorod catalysts was fabricated. Driven by the doped Pt atom, the catalyst solves the key kinetic problem about insufficient proton feeding in the process of nitrogen reduction, and actively transfers protons to intermediates of the hydrogenation steps in NRR. Moreover, the as-prepared catalyst presents the highest NH 3 yield value of 10.22 μg h −1 cm −2 among multitudinous Fe based catalysts at lower potential of −0.05 V ( vs . RHE) with an excellent Faraday efficiency (FE) of 15.3 %, which is higher than FeP/C without the Pt-driven proton-feeding effect, and the cathodic current density presents no significant change within 50 h. In addition, the density functional theory (DFT) and Attenuated total reflection surface-enhanced infrared absorption spectrum (ATR-SEIRAS) results verify the reaction path and protons-feeding kinetic process.
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ACS Catalysis
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2021
·
IF 13.084
Yu Gu,Shibin Wang,Huaijie Shi,Jun Yang,Suiqin Li,Haiyang Zheng,Wenbin Jiang,Jia Liu,Xing Zhong,Jianguo Wang
Environment-friendly electrochemical ozone production (EOP) is a promising route for in situ sterilization and discoloration applications. Herein, a Pt-SAs/BNC catalyst with Pt single atoms embedded into B/N codoped nanotubes is rationally designed and prepared. The process provides a local environment rich in oxygen intermediates and hence improves the EOP performance in neutral media by influencing the EOP thermodynamics and kinetics. The Pt-SAs/BNC catalyst exhibits excellent EOP performance with a Faraday efficiency of 21% at the current density of 50 mA cm–2, which is almost twice as much as that of commercial β-PbO2. Density functional theory calculations further reveal the synergistic effect between the B sites and the Pt single atom of the EOP mechanism. In addition, the Pt-SAs/BNC catalyst presented a significant performance in electrodegradation of various pesticides and antibiotics, indicating the potential environmental application capabilities of Pt-SAs/BNC.
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DALTON TRANSACTIONS
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2021
·Vol. 50
·期 27
·9529-9539
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IF 4.39
Xin Guo,Lina Kong,Jianping Xu,Jing Chen,Lan Li
Surface decoration of noble-metal cocatalysts on graphitic phase carbon nitride (g-C3N4) with high efficiency and trace content for water splitting is exciting but difficult to achieve. Herein, we report the anchoring of Au and metallic/oxidized Pt nanoparticles (NPs) on g-C3N4 as cocatalysts via a photoreduction process for enhancing photocatalytic H2 production. Au NPs are preferentially decorated on g-C3N4, which can control the formation of metallic/oxidized Pt complex species. The well dispersed Au and metallic/oxidized Pt NPs improved the light-harvesting and the photo-generated carrier separation of g-C3N4. G-C3N4 sequentially decorated with Au (0.3 wt%) and metallic/oxidized Pt (0.3 wt%) cocatalysts, exhibited the highest and stable H2 evolution rates of 2560 and 139 μmol h−1 g−1 under simulated sunlight and visible light (λ ≥ 420 nm) irradiation, respectively, compared to the samples that are simultaneously and sequentially decorated with the same content of Pt and Au on g-C3N4. The enhanced photocatalytic activity is attributed to the synergistic effect of Au and metallic/oxidized Pt cocatalysts, i.e., the effective localized surface plasma resonance coupling between Pt and Au NPs, as well as electron-sink function of metallic Pt, which promote the generation and transfer of more carriers from g-C3N4 to the Pt species, in addition to the superior hydrogen evolution capacity of metallic and oxidized Pt. This work maximizes the performance of noble-metal cocatalysts with minimized content and provides the possibility of realizing efficient solar-to-fuel conversion.
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高影响因子
ANALYST
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2020
·Vol. 146
·期 3
·956-963
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IF 3.978
Jun Ma,Gege Feng,Ying Ying,Yong Shao,Yongxin She,Lufei Zheng,A. M. Abd EI-Aty,Jing Wang
Herein, an indirect SERS sensing assay was developed for the determination of glyphosate (Gly) in tap water. The mechanism of detection was based on relieving the inhibitory effect of L-cysteine (L-cys) on a Au–Pt nanozyme by combining Gly with L-cys through divalent copper ions (Cu2+). In this method, a novel nano-chain-like Au–Ag composite with good repeatability was successfully fabricated to detect SERS signals of oxTMB without disturbing TMB Raman signals. Under optimal conditions, the SERS signal intensity of oxTMB (at 1605 cm−1) was proportional to the concentration of Gly. The results showed a good linear response over the concentration ranges of 10 μg L−1 to 1000 mg L−1. The limit of detection and limit of quantitation of Gly were found to be 5 μg L−1 and 10 μg L−1, respectively. In addition, good anti-interference ability against interfering cations and structural analogues deserves to be mentioned. This SERS assay can be used for detection of Gly in tap water that can meet the needs of practical detection.
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高影响因子
JOURNAL OF POWER SOURCES
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2020
·
IF 8.247
Junjie Ding,Weiling Hu,Li Ma,Mengyu Gan,Fei Xie,Wang Zhan,Wei Lu
Herein, through a simple and environmentally benign mechanical lapping, synchronous phosphorization pyrolysis and NaBH 4 reduction procedure, we have successfully constructed a novel nanoarchitecture, which confines bimetallic phosphides (NiCoP x ) within mesoporous carbon as Pt support for the first time (Pt/NiCoP x @NCNT-NG). Unlike conventional naked transition metal phosphides/carbon hybrids supports, the NiCoP x is encapsulated by graphene shells, in spite of without immediate contact, the electron interactions between NiCoP x and Pt outperform its monometallic phosphide counterparts. Benefiting from the synergistic effect between Pt, NiCoP x and mesoporous carbon, the Pt/NiCoP x @NCNT-NG reveals increased active sites and enhanced intrinsic activity of per active site, resulting in better catalytic activity and stability for methanol oxidation reaction . What's more, owing to the protection of the encapsulation carbon layer , the co-catalytic effect of NiCoP x can be well maintained after a long-time exposure. The present work provides a simple avenue to combine transition metal phosphides with mesoporous carbon and sheds new light into the development direction of transition metal phosphides for electrocatalysis .
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Catalysts
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2020
·Vol. 10
·期 10
·1192
·
IF 3.52
Jun Yan,Longlong Shan,Xiaoli Gu,Xingguang Zhang,Junmeng Cai
Three series of catalysts consisting of gold (Au), platinum (Pt), or gold-platinum bimetallic nanoparticles (NPs) with controlled sizes (Au NPs 10 ± 2 nm, Pt NPs 6 ± 2 nm) anchored on hierarchical micro-/meso-/macroporous silica were successfully developed and systematically evaluated for the selective oxidation of aromatic alcohols to their corresponding aldehydes. The catalysts were prepared by the sol-immobilization method using as-made Au NPs and/or Pt NPs colloids; the silica supports were prepared with controlled pore structures and the hierarchical porous structures of catalysts were created by controllable desilication via the alkaline solution of the metal colloids. The catalysts were characterized by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM), X-ray Photoelectron Spectroscopy (XPS), and Inductively Coupled Plasma-Mass Spectrometry (ICP-MS), and these results showed no synergistic effect between Au and Pt on boosting the catalytic performance, whereas they demonstrated a clear dependence of catalytic conversions and reaction rates on the structural porosity of Au-Pt bimetallic catalysts. Our findings could potentially inspire peer researchers and scientists to develop designer porous catalysts and processes in the selective organic conversions.Keywords:steric effect;Au-Pt catalysts;alcohol oxidation;hierarchical porous silica
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ENERGY & FUELS
·
2020
·
IF 3.421
Ruihan Luo,Xiuge Zhao,Honghui Gong,Wei Qian,Difan Li,Manyu Chen,Kai Cui,Jiajia Wang,Zhenshan Hou
Hydrogenolysis of glycerol to propanols is highly promising for the sustainable development of biomass refining. In this work, modified amorphous zirconium phosphate (ZrP)-supported Pt catalysts were developed and characterized thoroughly by X-ray diffraction, temperature-programmed desorption of ammonia, Fourier transform infrared spectra of adsorbed pyridine, temperature-programmed reduction, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, and Brunauer–Emmett–Teller surface area. The as-obtained catalysts were employed for selective glycerol hydrogenolysis to 1-propanol (1-PO) in a fixed-bed reactor. Owing to the incorporation of WOx, both the total acidity and the dispersion of Pt nanoparticles were enhanced significantly. The Pt/7WOx-ZrP catalyst could afford 81% yield of 1-PO at full conversion of glycerol in a long-term catalytic stability test (at least 70 h reaction time) and was regenerated by calcination in air. The results of the catalytic activity test and catalyst characterization indicated that the acid sites of the catalysts promoted the selective dehydration of glycerol into acrolein, whereas the Pt sites facilitated H2 dissociation and a sequential hydrogenation of acrolein into 1-PO.
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Nano Energy
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2020
·
IF 16.602
Qi Wang,Guang-Jie Xia,Zhi Liang Zhao,Yuanmin Zhu,Xiaobo Shi,Limin Huang,Yang-Gang Wang,Meng Gu
The carbon monoxide (CO) interaction effect on active Pt-based catalysts is critical because the surface reconstruction and phase separation behavior of bimetallic catalysts in a CO environment can profoundly impact the catalysts’ activity and durability. However, because direct and dynamic observation has proven elusive, the exact failure mechanisms of the nanocrystal structural modifications induced by CO are poorly understood. In this work, we probe the dynamic structural and compositional transformations of an individual PtPb@Pt nanoplates in a CO gas atmosphere via in-situ environmental transmission electron microscopy (ETEM) and confirmed with theoretical calculations. The interaction of Pt and Pb atoms with CO molecules are revealed dynamically, including the resulting breakdown of the PtPb@Pt nanoplates. The Pt atoms aggregate on surface facets of the original PtPb lattice and the Pt-CO complex mobilizes, cracking the Pt surface layers and stripping Pb atoms from the PtPb alloy core to form Pb(CO) 4 . These interactions provide direct clues for the failure analysis of the catalyst and, thus, represent a critical step towards the design of an anti-CO interaction catalyst.
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Catalysis Science & Technology
·
2020
·Vol. 10
·期 15
·5048-5059
·
IF 5.721
Yao-Yao Wang,Zheng Tang,Xue-Yang Ji,Song Wang,Zi-Shuo Yao,Jun Tao
Pt nanoparticles (NPs) can enhance the photocatalytic performance of metal–organic frameworks (MOFs) for hydrogen evolution. However, Pt atoms in the core of Pt NPs cannot be utilized for the hydrogen evolution reaction (HER) and the agglomeration of Pt NPs also reduces the enhancement effect. In this paper, we propose a simple and kinetically modulated post-synthetic strategy to encapsulate low-coordinated and monodispersed Pt clusters (PCs) with a mean size of 1.6 nm into the inner space of NH2-UiO-66 (U6N). The X-ray absorption spectroscopy (XAS) data indicate that the PCs with low coordination numbers and short Pt–Pt bonds possess more unoccupied d orbitals, which enhance the interactions between PCs and the MOF. Consequently, such enhanced interactions result in the acceleration of electron–hole separation that is beneficial to the HER activity of U6N, as confirmed by ultrafast transient absorption spectra. This MOF with encapsulated PCs shows a H2 production efficiency of 36.83 mmol h−1 g−1 and turnover number of 598 h−1 under visible light with photosensitizer erythrosin B and sacrificial agent triethanolamine. The results suggest that such PCs can efficiently boost the photocatalytic HER of U6N, and our strategy may provide a new avenue for fabricating MOFs with excellent catalytic properties.
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