RSC Advances
·
2024
·Vol. 14
·期 18
·12593-12599
·
IF 3.9
Junwei Li,Hongshuai Yin,Sisi Liu,Chaofa Xu,Zhixiong Cai
The catalytic performance of a catalyst is significantly influenced by its ability to activate hydrogen. Constructing frustrated Lewis pairs (FLPs) with the capacity for hydrogen dissociation on non-reducible supports remains a formidable challenge. Herein, we employed a straightforward method to synthesize a layered AlOOH featuring abundant OH defects suitable for constructing solid surface frustrated Lewis pair (ssFLP). The results indicated that the AlOOH-80 (synthesized at 80 °C) possessed an appropriate crystalline structure conducive to generating numerous OH defects, which facilitated the formation of ssFLP. This was further evidenced by the minimal water adsorption in the AlOOH-80, inversely correlated with the quantity of defects in the catalyst. As expected, the Pd loaded onto AlOOH (Pd/AlOOH-80) exhibited excellent catalytic activity in hydrogenation reactions, attributed to abundant defects available for constructing ssFLP. Remarkably, the Pd/AlOOH-80 catalyst, with larger-sized Pd nanoparticles, displayed notably superior activity compared to commercial Pd/Al2O3 and Pd/C, both featuring smaller-sized Pd nanoparticles. Evidently, under the influence of ssFLP, the size effect of Pd nanoparticles did not dominate, highlighting the pivotal role of ssFLP in enhancing catalytic performance. This catalyst also exhibited exceptionally high stability, indicating its potential for industrial applications.
研究领域:
催化化学
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材料科学
·
表面化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2017
·
IF 3.387
Xueliang Cui,Yunfeng Zheng,Meng Tian,Zhengping Dong
A novel yolk–shell-structured material (Fe 3 O 4 @γ-AlOOH-YSMs) with hierarchical γ-AlOOH flakes as the mesoporous shell and Fe 3 O 4 nanoparticles (NPs) in the hollow core was prepared by using Fe 3 O 4 @SiO 2 NPs as the seeds as well as NaAlO 2 and urea as the precursor. The prepared Fe 3 O 4 @γ-AlOOH-YSMs were used as a catalyst support for fabricating a Pd/Fe 3 O 4 @γ-AlOOH-YSMs nanocatalyst with no obvious aggregation of the Pd NPs. The Pd/Fe 3 O 4 @γ-AlOOH-YSMs nanocatalyst was utilized for the catalytic reduction of the widely used and highly toxic 4-nitrophenol, rhodamine B, methylene blue, and methyl orange; and showed excellent catalytic activity as compared with other noble-metal-based catalysts. Furthermore, the Pd/Fe 3 O 4 @γ-AlOOH-YSMs nanocatalyst also can be easily separated from the reaction mixture and reused for at least ten times without any obvious decrease in the catalytic activity, indicating its reusability and stability.
研究领域:
材料科学
·
环境化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Lanlan Shi,Xiaojun Wang,Feike Zhang,Jingxian Li,Yuanming Liu,Weijie Fu,Shuyun Yao,Shiyu Wang,Kang Ji,Yingjie Ji,Zhiyu Yang,Liwen Zhang,Jiangzhou Xie,Yi-Ming Yan
Palladium metal catalysts have emerged as the preferred choice for alkaline formate oxidation reaction (FOR) due to their high activity. However, their strong binding with adsorbed H (Had) allows Had to occupy the active site, resulting in slow FOR kinetics. Herein, we developed a ZrO2/Pd/C catalyst to decrease the Had binding strength on Pd active sites, thereby enhancing the FOR in alkaline media. Through experimental investigations and density functional theory (DFT) calculations, we elucidated the relationship between the d-band center of Pd and hydrogen binding energy (HBE). Our findings reveal that electron transfer from ZrO2 to Pd, driven by the work function disparity, results in a downshift of the d-band center of Pd. This shift weakens the HBE at Pd active sites, facilitating the desorption of Had intermediates and thereby improving catalytic efficiency. As a result, the ZrO2/Pd/C catalyst demonstrated a 2.8-fold increase in activity over commercial Pd/C, exhibiting a lower peak potential and a significantly higher peak current of 1787 mA mg–1. This work advances our understanding of the interplay between electronic structure and catalytic performance, setting a benchmark for high-performance electrocatalysts in energy conversion technologies.
研究领域:
催化
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电化学
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材料科学
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能量转换
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产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2024
·Vol. 99
·期 4
·978-988
·
IF 2.8
Likai Dai,Zheng Fang,Anxian Peng,Yunhong Chen,Yitong Liu,Huimei Chen,Rongjun Yan,Rencheng Zhou,Mingming Du
BACKGROUND Photothermal catalytic oxidation technology for synthesis of high value-added chemicals has become a hot topic of research at home and abroad. As a special structure, titania (TiO 2 ) nanotubes (Ti-NTs) possess larger specific surface area and adsorption capacity, which have shown great application prospects in photothermal catalytic oxidation. RESULTS In this work, high-performance palladium (Pd-Ti-NTs catalyst were prepared and applied to the photothermal catalytic oxidation of 5-hydroxymethyl (HMF) and benzyl alcohol. The photothermal dependence on catalytic activity and selectivity of HMF and benzyl alcohol oxidation was studied in detail. The results revealed that compared with thermal catalytic oxidation, the catalysts showed significantly higher conversions of both benzyl alcohol and HMF under light. in particular, HMF conversion increase from 55.6% to 99.7%. Aldehyde oxidation is inhibited by alcohol and can be dramatically promoted by light radiation. This is probably because alcohol can inhibit the adsorption of aldehyde, and this inhibiting effect is weakened through light radiation, thus promoting the oxidation of aldehydes. Therefore, the selectivity of the final products 2,5-furandicarboxylic acid (FDCA) and benzoic acid were dramatically increased in both systems under light radiation, and the selectivity for FDCA was obviously increased from 5.8% to 61.3%, and the yield reached 61.0%, which is higher than that of most of the reported Pd-TiO 2 -based catalysts for FDCA. CONCLUSIONS In this paper, we verify that Pd-Ti-NTs could preferentially promote the conversion of aldehydes to acids in the presence of light, and obtained catalysts with high catalytic performance and high stability for benzyl alcohol and HMF oxidation. © 2024 Society of Chemical Industry (SCI).
研究领域:
催化
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材料科学
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化学工程
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2025
·
IF 4.7
Qingfang Jiang,Wujian Zhang,Weijian Ge,Yiping Jin,Wenfeng Han,Ying Li,Haodong Tang
Sintering deactivation of loaded precious metal catalysts is a pressing issue in the field, significantly reducing catalyst activity. Among them, the redispersion of carbon-loaded precious metal catalysts under a high-temperature atmosphere suffers from the problem of carbon carriers being prone to carbonization. In this study, the sintered PdZn/AC catalysts could be redispersed at low temperatures by adding the additive Zn. Combined with TEM, XRD, XPS, and other characterization means, it was found that the main reason for the redispersion of the sintered catalysts was that the Zn additive could form an alloy with Pd, which promoted the formation of high-valent Pd species, which exfoliated into small particles by oxidation in the O 2 –CO atmosphere. In addition, the factors that influenced the process (Zn content, redispersion temperature, treatment time, and number of treatments) were investigated using the controlled variable method. The present work presents a new idea for recycling sintered precious metal catalysts.
研究领域:
催化化学
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材料科学
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化学工程
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表面化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Wei Xiong,Lin Qi,Ning Jiang,Qi Zhao,Lingxiao Chen,Xin Jiang,Yuan Li,Zaigang Zhou,Jianliang Shen
Photodynamic therapy (PDT) is a promising strategy for cancer treatment. It can not only generate reactive oxygen species (ROS) to cause the chemical damage of tumor cells in the presence of enough oxygen but also promote the antitumor immunity of T cells through enhancing the production of interferon γ (IFN-γ). However, one phenomenon is ignored so far that the enhanced production of IFN-γ caused by PDT may significantly increase the expression of programmed death-ligand 1 (PD-L1) on the tumor cell membrane and thus could inhibit the immune killing effects of T cells. Herein, we report the construction of a composite by loading metformin (Met) and IR775 into a clinically usable liposome as a two-in-one nanoplatform (IR775@Met@Lip) to solve this problem. The IR775@Met@Lip could reverse tumor hypoxia to enhance ROS production to elicit more chemical damage. Besides, the overexpression of PD-L1 by PDT was also effectively down-regulated. These therapeutic benefits including decreased PD-L1 expression, alleviated T cell exhaustion, and reversed tumor hypoxia successfully suppressed both the primary and abscopal tumor growth in bladder and colon cancers, respectively. Combining with its excellent biocompatibility, our results indicate that this IR775@Met@Lip system has great potential to become a highly effective cancer therapy modality.
研究领域:
癌症研究
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药学
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免疫治疗
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纳米技术
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生物医学工程
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF RARE EARTHS
·
2025
·
IF 7.2
Jiaman Wang,Jing Xiong,Zekai Cui,Yuanfeng Li,Hao Guo,Guilin Liu,Yaxiao Ma,Linsheng Xu,Jinqing Jiao,Jianping Zou,Yuechang Wei
CeO 2 , a pivotal rare earth oxide in environmental catalysis, has garnered extensive interest for soot oxidation owing to its exceptional oxygen storage capacity and oxygen vacancy-rich surfaces. To further optimize catalytic efficiency, we engineered spherical CeO 2 with exposed (111) facets via hydrothermal synthesis and uniformly anchored Pd species through a gas bubbling-assisted membrane reduction (GBMR) strategy. The formation of Pd–O–Ce interfacial units is identified as critical active sites, where metal-support interaction (MSI) significantly enhances oxygen transfer. Notably, the Pd 1.0 /CeO 2 catalyst achieves a remarkable T 50 of 356 °C (14% lower than pristine CeO 2 ), attributed to highly dispersed Pd species and abundant Pd–O–Ce interfaces. In contrast, excessive Pd species loading induces particle agglomeration, weakening MSI effect and catalytic performance. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional thoery (DFT) calculations reveal that the Pd–O–Ce interface promotes NO adsorption – the rate limiting step – by generating electron-rich Pd sites and oxygen vacancies, thereby accelerating NO-to-NO 2 conversion and subsequent soot oxidation. This work highlights the pivotal role of interfacial engineering in optimizing Pd–CeO 2 catalysts, offering a rational design strategy for high-performance soot oxidation systems in diesel emission control.
研究领域:
环境催化
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材料科学
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多相催化
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排放控制
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纳米材料
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2016
·
IF 5.31
Zhiqiang Zhang,Yongpeng Xu,Wenxin Shi,Wei Wang,Ruijun Zhang,Xian Bao,Bing Zhang,Li Li,Fuyi Cui
The Pd–Cu/γAl 2 O 3 catalysts were prepared by impregnation method and introduced into the cathode chamber of a divided electrochemical denitrification cell with two graphite plates as the cathode and anode, to enhance the nitrate removal efficiency and N 2 selectivity. The Pd–Cu/γAl 2 O 3 catalysts were characterized by transmission electron microscope (TEM), X-ray diffraction (XRD), specific surface area measurements (BET) and inductively coupled plasma-atomic emission spectrometry (ICP-AES). In the rationally designed electrochemical-catalytic (ECC) system, the as-prepared catalyst could significantly enhance the nitrate degradation rate to 1.08 mg/L at current density of 10 mA/cm 2 , which was approx. 2.5 times compared with the electrochemical (EC) system without catalysts adding in. Additionally, a higher nitrogen selectivity of 80.37% was obtained under the same experiment condition. The improved performances were likely due to the presence of a catalytic reduction reaction of nitrate with the appropriate amount of hydrogen generated by electrolysis as reductant. Significantly, the current efficiency was calculated and enhanced value of 20–40% (depended on current density) was obtained in the ECC process with a catalyst content of 1.0 g/L.
研究领域:
环境科学
·
电化学工程
✓ 已验证
产品关联
DOI
高影响因子
iScience
·
2024
·
IF 4.6
Chenliang Zhou,Shaoyuan Shi,Xingyu Zhang,Yuting Sun,Guan Peng,Wenjing Yuan
Constructing platinum-like materials with excellent catalytic activity and low cost has great significance for hydrogen evolution reaction (HER) during electrolysis of water. Herein, palladium nanoparticles (NPs) deposition on the surface of Co NPs using nitrogen-doped carbon (NC) as substrate, denoted as N-ZIFC/CoPd-30, are manufactured and served as HER electrocatalysts. Characterization results and density functional theory calculations validate that Pd-Co heterojunctions with NC acting as “electron donators” promote the Pd species transiting to the electron-rich state based on an efficient electron transfer mechanism, namely the N-C polar bonds induced strong metal-support interaction effect. The electron-rich Pd sites are beneficial to HER. Satisfactorily, N-ZIFC/CoPd-30 have only low overpotentials of 16, 162, and 13 mV@-10 mA cm −2 with the small Tafel slopes of 98 mV/decade, 126 mV/decade, and 72 mV/decade in pH of 13, 7, and 0, respectively. The success in fabricating N-ZIFC/CoPd opens a promising path to constructing other platinum-like electrocatalysts with high HER activity.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Yingfang Zhu,Sihao Wang,Qingyu Luo,Haifu Huang,Shaolong Tang,Youwei Du
Developing electrocatalysts with high-Pt-utilization efficiency and appropriate surface oxygen affinity through a facile and scalable route is urgently needed for proton exchange membrane fuel cells. Here, SPD-annealing strategy is demonstrated to prepare ordered low-Pt-loading Pd–Pt–Fe nanoalloys with an average particle size of less than 5 nm and excellent electrocatalytic performance. Furthermore, the ORR performances of Pd–Pt–Fe/C nanoalloy catalysts are rationally modified by means of both precise composition control and structural transformation. With an optimal component proportion, the prepared Pd 0 . 75 Pt 0 . 25 Fe/C catalyst exhibits the most excellent intrinsic activity due to the synergistic interaction of lattice strain and ligand effect. Benefiting from the compressive strain effect induced by the relatively tight arrangement of the ordered structure, the adsorption energy of the intermediate oxygen-containing species is effectively weakened, enabling the Pd 0 . 75 Pt 0 . 25 Fe/C to obtain enhanced ORR catalytic performance in acidic condition. Notably, compared with the disordered Pd 0 . 75 Pt 0 . 25 Fe/C, the ordered Pd 0 . 75 Pt 0 . 25 Fe/C shows an extremely superior stability of 98.5% mass activity retention after 10 000 cycles. This work could provide a facile and versatile approach to constructing the ordered low-platinum electrocatalysts with enhanced ORR properties.
研究领域:
材料科学
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电化学
·
能源科学
✓ 已验证
DOI
高影响因子
Environmental Science-Nano
·
2020
·Vol. 7
·期 5
·1566-1581
·
IF 7.683
Zimo Lou,Zheni Wang,Jiasheng Zhou,Chuchen Zhou,Jiang Xu,Xinhua Xu
Electrocatalytic hydrodechlorination (ECH) has been proposed as a potential technology for the effective degradation of organochlorine contaminants. In this study, a nanoscale Pd/TiC catalyst with low resistance was dip-coated onto Ti, aiming to fabricate a stable Pd/TiC/Ti electrode with enhanced ECH reactivity for efficient dechlorination. Electrochemical techniques indicated that the Pd/TiC/Ti electrode had a larger electrochemically active surface area and more rapid interfacial charge transfer than the conventional Pd/C/Ti electrode. In a batch experiment, the dechlorination rate for ECH of 2,4-dichlorobenzoic acid (2,4-DCBA, a model pollutant) by Pd/TiC/Ti was 1.3–14.5 times higher than those by Pd/C/Ti, Pd/MWCNTs/Ti, and Pd/MoS2/Ti, respectively. Scavenger experiments, ESR spin-trapping spectroscopy, and cyclic voltammetry clarified the intensified atomic H* generation by Pd/TiC/Ti. DFT calculations revealed that Pd/TiC/Ti had stronger binding ability with atomic H* (Eads: −2.89 eV vs. −2.44 eV) and 2,4-DCBA (Eads: −3.62 eV vs. −2.15 eV), respectively, when compared with Pd/C/Ti. As a result, enhanced generation of atomic H*, together with strengthened adsorption of atomic H* and 2,4-DCBA, would contribute to a faster ECH reaction. The Pd/TiC/Ti electrode retained its reactivity after 10 successive batch experiments (80 h), and showed high tolerance to the constituents in actual water matrices including lake water and river water. This study proposed a promising ECH electrode for the treatment of chlorinated organics in water matrices.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Hualei Wang,Cong Xi,Huiming Yin,Yi Ding
Conventional strategies for developing highly efficient electrocatalysts involve enhancing thermodynamics to minimize overpotential and improving kinetics to maximize reaction current. However, current research on Pd-based catalysts for formic acid oxidation reaction (FAOR) mainly focuses on accelerating its kinetics to increase the peak current. This study proposes a catalyst design that can simultaneously improve the kinetics and thermodynamics of FAOR. Specifically, the home-made catalyst (NPG-Pt 1 -Pd 1 ) is obtained by sequentially depositing monolayer Pt and Pd shells on the surface of nanoporous gold (NPG) substrate. Compared with commercial Pd/C, this electrocatalyst exhibits a noticeable negative shift in onset potential (∼100 mV) and a significantly improved peak current (∼6 times). Experimental data and theoretical calculations demonstrate that NPG-Pt 1 -Pd 1 exhibits a comparatively suitable adsorption energy for small molecules, not only reducing the overpotential but also accelerating the reaction rate of FAOR. Moreover, when applied in direct formic acid fuel cells (DFAFC), the NPG-Pt 1 -Pd 1 anode with an exceptionally low Pd loading of 8.5 μg cm −2 , achieves a remarkable power density of 141 mW cm −2 . The power efficiency of Pd is 230 times that of Pd/C (1 mg cm −2 , 73 mW cm −2 ). Therefore, this work provides a new methodology for developing efficient Pd-based FAOR electrocatalysts .
研究领域:
材料科学
·
电化学
✓ 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）