Molecular Catalysis
·
2023
·
IF 4.6
Yanlin Xu,Zhuoyi Liu,Bin Liu,Bin Dong,Yuan Pan,Yanpeng Li,Yichuan Li,Hailing Guo,Yongming Chai,Chenguang Liu
Transformation of lignin-derived feedstocks into valuable hydrocarbons is of significant importance but still challenging. This work investigates the hydrodeoxygenation (HDO) of lignin compound guaiacol on Pt-based catalysts with improved surface hydrophobicity and metal dispersion for the first time. The efficiency of guaiacol hydrodeoxygenation into hydrocarbons over Nb 2 O 5 -modified Pt-based catalyst reaches 51 %, nearly doubling that over unmodified Pt/γ-Al 2 O 3 catalyst (25 %). On the one hand, Nb 2 O 5 causes the decrease of hydroxyl groups on catalyst, leading to the enhanced hydrophobicity of catalysts, which increases the reaction rate of guaiacol into hydrocarbons on unit of Pt metal sites. On the other hand, Nb 2 O 5 strengthens the metal-support interaction, which minimizes the size of Pt nanoparticles, providing more exposed metal sites, thus leading to a higher hydrocarbons yield on catalyst. However, excess introduction of Nb 2 O 5 leads to partial coverage of Pt metal sites, resulting in decreased yield of hydrocarbons. Furthermore, the routes of guaiacol HDO reaction over modified Pt-based catalysts are investigated. This work further illustrates the influence of catalyst surface properties on the HDO process of lignin compound, and thereby provides a promising approach for adjustment of catalyst surface properties in order to promote water-liberated reactions.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Lifang Yang,Jiangju Si,Liang Liang,Yunfei Wang,Li Zhu,Zizhong Zhang
Photocatalytic water splitting has been identified as a promising solution to tackle the current environmental and energy crisis in the world. However, the challenge of this green technology is the inefficient separation and utilization of photogenerated electron-hole pairs in photocatalysts. To overcome this challenge in one system, a ternary ZnO/Zn 3 In 2 S 6 /Pt material was prepared as a photocatalyst using a stepwise hydrothermal process and in-situ photoreduction deposition. The integrated S-scheme/Schottky heterojunction in the constructed ZnO/Zn 3 In 2 S 6 /Pt photocatalyst enabled it to exhibit efficient photoexcited charge separation/transfer. The evolved H 2 reached up to 3.5 mmol g -1 h - 1 . Meanwhile, the ternary composite possessed a high cyclic stability against photo-corrosion under irradiation. Practically, the ZnO/Zn 3 In 2 S 6 /Pt photocatalyst also showed great potential for H 2 evolution while simultaneously degrading organic contaminants like bisphenol A. It is hoped in this work that the incorporation of Schottky junctions and S-scheme heterostructures in the construction of photocatalysts would lead to accelerated electron transfer and high photoinduced electron-hole pair separation, respectively, to synergistically enhance the performance of photocatalysts.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS ES&T Engineering
·
2023
·
IF 7.1
Haifang Mao,Mengli Xu,Shuangjun Li,Yuqing Ren,Yun Zhao,Jun Yu,Qizhong Zhang,Wenshu Zhao,Gui Zhang,Lan Yan,Zhenmin Xu,Zhenfeng Bian
The activation of surface lattice oxygen is crucial for designing highly efficient photocatalysts for volatile organic compound (VOC) purification. Herein, the Pt/TiO2–x catalyst with abundant oxygen vacancies was successfully prepared via the pyrolysis of the Pt-modified Ti metal–organic framework (MOF) under an air atmosphere. Detailed experimental results and density functional theory calculations revealed that the introduction of oxygen vacancies modulated the electronic configuration of the Pt site and enhanced the charge transfer from Ti to Pt, which created an electronic metal–support Pt–Ti interaction interface (EMSI). The established Pt–Ti interface is favorable for the activation of the surface lattice oxygen adjacent to the Pt site [identified by H2 temperature-programmed reduction (TPR), electron paramagnetic resonance (EPR), and in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS)] and subsequently facilitates toluene oxidation via a direct ring opening process. This study offers a promising strategy for the design of high-performance photocatalysts for VOC oxidation.
✓ 已验证
产品关联
DOI
高影响因子
Green Energy & Environment
·
2022
·
IF 12.781
Yang Zhou,Lice Yu,Jinfa Chang,Ligang Feng,jiujun Zhang
Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique, and highly efficient bifunctional catalysts for membrane electrode fabrication are required to drive the electrolysis reactions. Herein, the efficient catalytic promotion effect of a novel catalyst promoter, CoTe, on Pt is demonstrated for low carbon alcohol fuels of methanol and ethanol electrolysis for hydrogen generation. Experimental and density functional theory calculation results indicate that the optimized electronic structure of Pt–CoTe/C resulting from the synergetic effect between Pt and CoTe further regulates the adsorption energies of CO and H∗ that enhances the catalytic ability for methanol and ethanol electrolysis. Moreover, the good water activation ability of CoTe and the strong electronic effect of Pt and CoTe increased the tolerance ability to the poisoning species as demonstrated by the CO-stripping technique. The high catalytic kinetics and stability, as well as the promotion effect, were also carefully discussed. Specifically, 71.9% and 75.5% of the initial peak current density was maintained after 1000 CV cycles in acid electrolyte for methanol and ethanol oxidation; and a low overpotential of 30 and 35 mV was required to drive the hydrogen evolution reaction in methanol and ethanol solution at the current density of 10 mA cm −2 . In the two-electrode system for alcohol fuels electrolysis, using the optimal Pt–CoTe/C catalyst as bi-functional catalysts, the cell potential of 0.66 V (0.67 V) was required to achieve 10 mA cm −2 for methanol (ethanol) electrolysis, much smaller than that of water electrolysis (1.76 V). The current study offers a novel platform for hydrogen generation via low carbon alcohol fuel electrolysis, and the result is helpful to the catalysis mechanism understanding of Pt assisted by the novel promoter.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Gongguo Zhang,Yingying Wang,Feng Liu,Yuhan Kong,Maochang Liu,Yiqun Zheng
We report the fabrication of “Pt-on-PdAg” heterogeneous nanocrystals in the form of trigonal/hexagonal plate (THNPs) and explored their applications in electroxidation of methanol (MOR) in alkaline medium. In particular, PdAg polyhedral nanoparticles are prepared in advance, followed by the addition of Pt salts to allow in situ galvanic replacement reaction (GRR) between them, leading to the formation of Pt nano-islands on PdAg particle surface and the transformation of the overall morphology into trigon/hexagon. The deliberately designed Pt-“PdAg alloy” interface arising from the hybrid structure greatly enriches the absorption sites, showing noticeable structural advantages in MOR electrocatalysis . Particularly, the carbon-supported Pt-on-PdAg THNPs exhibit nearly 30-fold increase in specific activity as compared to that of commercial Pt/C, as well as enhanced reaction kinetics and long-term durability. DFT calculations suggest that the reaction of CH 3 OH oxidation mediated by PtAgPd is energetically more favorable compared to the similar reaction promoted by Pt, which rationalizes the experimental observation that PtAgPd shows the improved catalytic performance. The present study offers a feasible route to construct trimetallic nanocrystals with successful interface engineering, and validates their promising use as fuel cell electrocatalyst from both experimental validation and fundamental insights. It may help enlighten the rational design of heterostructured electrocatalysts with regulated multiple active sites.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Liuxuan Luo,Zehao Tan,Cehuang Fu,Rui Xue,Xiaojing Cheng,Tianzi Bi,Lutian Zhao,Yangge Guo,Xiyang Cai,Jiewei Yin,Shuiyun Shen,Junliang Zhang
Increasing the accessible active sites and especially improving the intrinsic activity are two major effective strategies for enhancing the electrocatalytic activity of nanomaterials. Accordingly, through the trioctylphosphine (TOP)-based CO-assisted solvothermal method and the small-amount Pt 2+ galvanic replacement, highly uniform Pd nanotetrahedrons (NTs) with Pt-doped surfaces are synthesized and supported onto carbon black. Comprehensive experimental and theoretical analyses reveal that, owing to the Pt surface-doped (SD) nanostructure, the conformal formation of surface Pt {111} facets, as well as the strain and electronic effects induced by the Pd–Pt alloy structure, Pd/ SD Pt NTs/C exhibits much better electrocatalytic performance than Pd NTs/C, commercial Pd/C, and Pt/C toward both oxygen reduction and formic acid oxidation reactions, showing greatly improved metal utilization and area/mass-specific activity. This study develops a high-performance bifunctional electrocatalyst, and firstly introduces TOP as the easy-removable surface-energy adjuster for the Pd shape-controlled synthesis, which may be further expanded to other metals and shapes.
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES B-BIOINTERFACES
·
2022
·
IF 5.999
Ruolan Zhou,Xiaohong Zhuang,Qiaoli Wu,Ming Jin,Chaochuan Zheng,Yayun Jiang,Yongliang Lou,Laibao Zheng
As an alternative to natural enzymes , artificial enzymes based on nanomaterials have attracted a lot of attention owing to their outstanding catalytic activity and high stability as well as low cost. Cu-MOF loaded with platinum nanoparticles (labeled Cu-MOF@Pt) was prepared by simple one-step wrapping method using platinum nanoparticles, copper nitrate trihydrate and 1,3,5-tricarboxybenzene. It was confirmed that Cu-MOF@Pt exhibits peroxidase-like activity, which can quickly catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) and produce blue oxidized TMB (oxTMB) in the presence of hydrogen peroxide (H 2 O 2 ). Additionally, steady-state kinetics showed that Cu-MOF@Pt exhibits stronger appetency to TMB and H 2 O 2 compared with horseradish peroxidase . Thanks to the peroxidase-like activity of Cu-MOF@Pt, a highly selective colorimetric method for glucose detection has been successfully established, the linear range is 2–15 mM (R 2 =0.9999) and the Limit of Detection (LOD) is 0.42 mM, with a detection range that meets clinical needs. Moreover, its good intra- and inter-assay precision and excellent stability make the results of glucose detection very reproducible. The detection performance of 90.09% was still maintained at 4 ℃ for 2 months. In conclusion, a new nanocomposite was successfully prepared and its selective detection ability for glucose was proved, which established a good basis for the clinical development of new enzymes for biosensors .
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Songbo Wang,Pengjie Liu,Chengzhen Meng,Yidan Wang,Lei Zhang,Lun Pan,Zhen Yin,Na Tang,Ji-Jun Zou
Photoelectrochemical (PEC) water splitting is a promising approach to solve the current energy and environmental crises. Herein, we developed a “one stone, two birds” strategy to construct Au@Pt decorated ZnO/CdS heterojunctions (ZCAP) with Au-S bond and surface plasmon resonance (SPR) effect for promoted PEC water splitting. The optimized ZCAP structure exhibited the highest photocurrent density of 4.23 mA/cm 2 at 1.23 V vs. RHE and hydrogen evolution rate of 72.3 μmol·cm −2 ·h −1 , which is magnitude higher than pure ZnO. In-depth investigations indicate that SPR effect can afford hot electrons, whereas Au-S bonds over interface act as transmission bridge for facilitated electron transfer, the synergy of them achieves efficient charge separation and light utilization. Meanwhile, surface Pt nanoparticles serve as active sites for rapid charge transfer and promoted surface reaction. This article illustrates that the synergy of SPR and electron transfer bridge is an efficient strategy for promoted PEC performance.
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2022
·
IF 5.518
Liang Cheng,Shuilai Qiu,Jing Wang,Weijian Chen,Jingwen Wang,Wenxiang Du,Lei Song,Yuan Hu
Human health is being seriously harmed by tumors. In order to obtain excellent anti-tumor effects, platinum (Pt) nanozyme-modified black phosphorus (BP) loading with L -Arginine (LArg) (BPPL) is prepared to realize nitric oxide (NO) therapy and sonodynamic therapy (SDT), achieving a synergistic effect to therapy. In this system, BP is utilized as the sonosensitizer. Pt can catalyze the decomposition of hydrogen peroxide (H 2 O 2 ) to produce oxygen (O 2 ) and relieve the hypoxic environment of tumor tissue. The increase in O 2 concentration is conducive to the generation of ROS under ultrasound (US) stimulation. The deposition of precious metals hinders the recombination of some electrons (e ) and holes (h + ), and further improves the yield of reactive oxygen species (ROS). LArg is employed as the exogenous NO supplementation. Under the stimulation of US and ROS, NO is generated to cause further cell apoptosis. Tests in vitro and in vivo have proved the great potential of the combination of SDT and gas therapy in tumor treatment.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Dandan Liu,Haiou Liang,Chunping Li,Jie Bai
Photocatalytic water splitting is a prospective strategy to solve the shortage of human fossil fuel energy. In this work, we designed and synthesized the Pt as co-catalyst decorated on TiO 2 nanotubes/metastable zinc-blende (ZB) CdS nanoparticles (NPs) with highly exposed (1 1 1) facets (HPTCA3) via the electrospinning-solvothermal and chemical deposition methods. The H 2 evolution rate of HPTCA3 was 15025.38 μmol·g −1 ·h −1 , which was about 111.3 and 2.4 times stronger than that of pure CdS power and Pt-TiO 2 /CdS hollow nanotubes (HPTC). The XRD patterns showed the presence of acetate promoted the growth of ZB CdS (1 1 1) crystal facets, and the photogenerated electrons were easily tended to accumulate on the CdS (1 1 1) facets, whichwas conducive to the transmission of electrons on the CdS and TiO 2 interface. The type II heterojunction can broaden the visible light response range and accelerate the separation and transfer of photo-generated electrons and holes which can be supported by the Optical and Electrochemical characterizations. Band structure calculations and XPS spectrum indicated that the composite catalyst had an efficient electron transfer mechanism, which was beneficial for the spatial separation of photogenerated carriers. The work provides a rational photocatalyst design to improve the performance of photocatalytic splitting of water into hydrogen.
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2022
·Vol. 14
·期 9
·3579-3588
·
IF 8.307
Jianjun Zhou,Tian Wang,Cheng Cheng,Fan Pan,Yunqing Zhu,Hongrui Ma,Junfeng Niu
Electrocatalytic oxidation is regarded as an effective technique for decomposing refractory organic compounds like perfluorooctanoic acid (PFOA). However, achieving highly efficient and long-life electrodes is still a great challenge. Herein, Ti/RuO2–IrO2@Pt anodes consisting of Pt4+ and Pt0 species were fabricated by combining modified microemulsion technology with a calcination process, in which Pt nanoparticles were highly dispersed and encapsulated in Ru–Ir composite oxides to form a strong metal–support interaction (SMSI) structure. The as-constructed SMSI layer on the Ti/RuO2–IrO2@Pt anode resulted in the improvement of the charge transfer capability and also increased the degradation (99.30%) and mineralization (91.32%) of PFOA during the electrochemical oxidation process. Notably, the service lifetime of Ti/RuO2–IrO2@Pt anodes was remarkably improved from 24 to 42.3 h compared to commercial Ti/RuO2–IrO2 anodes. Moreover, the possible degradation mechanism of PFOA was also speculated through the detection of short-chain perfluorocarboxylic acids and reactive radicals. These results not only revealed that the concept and methodology of SMSI could be an effective way for constructing highly efficient and stable electrocatalysts but also greatly advanced fundamental understanding.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING
·
2021
·Vol. 128
·期 1
·1-14
·
IF 2.584
Chen Peng,Wu Keliang,Peng Xiang,Ma Yue,Yang Xuqi,Duan Xinping,Ma Yan,Liu Zhiyong
Hydrogen and oxygen production based on photocatalytic monolithic water splitting is considered to be one of the effective ways to produce sustainable and clean energy. The key challenge in this process is to develop new photocatalysts that can simultaneously produce H 2 and O 2 at a stoichiometric ratio of 2:1 without the use of any sacrificial agents. In order to solve this problem, highly efficient and ingenious photosystems in nature have been studied intensively. Herein, we prepared printable Z-type composite photocatalysts CdS@TiO 2 /Pt/ITO/WO 3 /Co 3 O 4 mimicking biological vegetative leaves in nature and constructed an “artificial leaf” device that completely decomposes water. We use an electron solid penetrating transporter ITO, which can rapidly transfer photogenerated electrons and photogenerated holes and reduce the compound rate of photogenerated carriers. Thus, the efficiency of photocatalytic total water dissolution is enhanced. This photocatalyst was able to produce both H 2 and O 2 in water with an H 2 production rate of 75.93 μmol g −1 h −1 and an O 2 production rate of 36.49 μmol g −1 h −1 . We designed the oxygen-producing photocatalyst WO 3 /Co 3 O 4 , which produced oxygen at a rate of 159.21 μmol g −1 h −1 6 times higher than that of WO 3 alone. Furthermore, the morphology, composition, and microstructures of the photocatalyst were characterized by field-emission scanning electron microscopy, transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and nitrogen adsorption–desorption.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）