JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Qiong Wu,Lu Wang,Baozheng Zhao,Lang Huang,Shitao Yu,Arthur J. Ragauskas
A highly stable Pd-loaded N-doped carbon catalyst (ACN pd ) for phenol hydrogenation was prepared from chitosan by hydrothermal carbonization. ACN pd does not require a reduction step before catalytic use due to the Pd in the as-prepared catalyst mainly exists in the form of Pd 0 (80%). The carbon support involves N-containing groups such as pyridinic nitrogen and pyrrolic nitrogen, which could provide basic sites to adsorb phenol effectively. The as-fabricated ACN pd shows high catalytic performance with turnover frequency (TOF) of 29.34 h −1 . Accordingly, a phenol conversion of 100% and a cyclohexanone selectivity of 99.1% are achieved in 5 h at 100 °C and 1 MPa H 2 . This outstanding performance is attributed to the synergetic effects of the Pd particles, the N-functional groups, and the Lewis acid sites on the support. The carbon support presents intrinsic Lewis acid sites due to its electrophilicity, and Pd doping further increases the strength of such acid sites as it causes electron-deficient structural features. Moreover, the Lewis acid sites inhibit the over-hydrogenation from cyclohexanone to cyclohexanol. This study provides new insights into the application of functional biomass-based carbon materials as catalyst supports.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Guilin Wei,Junhong Luo,Wenwen Yong,Jiangfeng Song,Yan Shi,Xingwen Feng,Ning Liu
Controllable nuclear fusion is a major breakthrough in the future energy field and an important way for mankind to pursue clean and sustainable energy. However, since the fusion reaction raw material tritium is radioactive (β decay, half-life is 12.43 years), the leakage of these hydrogen isotopes under accident conditions will bring the risk of explosion and cause radiation damage to human. Therefore, efficient removal of hydrogen isotopes leaked due to accidents is crucial to the safe operation of nuclear fusion and human health. This study utilizes the metal-support interaction effect to design a series of Pd catalysts for efficient catalytic oxidation of hydrogen isotopes. Using pure silicon zeolite as a carrier, Pd is confined in the channel structure using a ligand-stabilized in situ encapsulation method. The prepared catalyst has nanoscale dispersed metal clusters and has excellent hydrogen isotope catalytic oxidation performance. This study systematically explored the effects of catalyst post-treatment methods, reaction space velocity, and reaction temperature on the hydrogen isotope catalytic oxidation conversion rate. The results show that the catalyst can be fully reduced at 600 °C and can achieve a hydrogen isotope catalytic oxidation conversion rate of greater than 98 % (24,000 mL g –1 h –1 ) at 100 °C. The conversion rate for hydrogen is higher than 96 % under the same space velocity at 50 °C. After 35,360 min (∼24.5 d) of continuous testing and intermittent operation, the catalyst can also maintain a conversion rate of 99 % (100 °C, 24,000 mL g –1 h –1 ). A lower reduction temperature will leave some organic matter, which will coordinate and bond on the Pd clusters and thus affect the catalytic activity. Under the same conditions, the hydrogen conversion rate of the catalyst directly reduced at 400 °C was 14 % lower than that of reduction at 600 °C, which proves the criticality of the reduction temperature. This work demonstrates a systematic study of utilizing the confinement effect of molecular sieve pores to obtain Pd cluster catalysts and applying them to the oxidative removal of hydrogen isotopes. It focuses on exploring the impact of the direct reduction temperature of the catalyst on its performance, which may be useful for providing a certain reference for designing relevant catalysts in engineering applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Xiao Liu,Yanjun Zhang,Wuxia Zhang,Gang Cheng,Fan Tian,Wei Li,Jinyan Xiong
Rapid charge recombination, limited light response, and slow surface reactions were observed in the photocatalysts, thereby limiting their future-oriented applications in photocatalytic hydrogen production through water splitting. Constructing a multi-channel charge separation photocatalysis system could solve those questions. In this study, Pd-TiO 2 -Cu 2 O composites were successfully accomplished via a facile chemical reduction method. The Pd-TiO 2 -Cu 2 O composite exhibited improved photocatalytic hydrogen production (13069.7 μmol g −1 h −1 ), which was over 6 times as much as that of pure TiO 2 . Based on the photo/electrochemical measurements, it was proposed that a Type II heterojunction was formed at the TiO 2 -Cu 2 O interface under light irradiation, and concurrently, a Schottky barrier was established between Pd and TiO 2 . Accordingly, the Type II heterojunction-created built-in electric field would facilitate the separation of photogenerated charges. Simultaneously, the introduction of Pd accelerates the accumulation of electrons and further enhances the charge transfer rate. The combination of such a Type II heterojunction and Schottky junction synergistically created a multi-channel charge separation system, optimizing surface reactions and thus improving photocatalytic efficiency. This work provided a rational approach for building efficient multi-component photocatalysis systems featuring Type II heterojunction/Schottky junction for photocatalytic hydrogen evolution.
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PubMed
高影响因子
ENERGY
·
2025
·
IF 9.4
Hao Sun,Hui Gao,Yanhua Li,Youchang Du,Jiao Wang,Huaizhi Han,Guice Yao,Dongsheng Wen
Fully utilizing the chemical heat sink generated by hydrocarbon fuel cracking is critical for enhancing the endothermic cooling capacity of the fuel. In this study, a catalytic strategy based on oil-dispersible palladium nanoparticles (Pd NPs) is proposed for the supercritical cracking of RP-3. Pd NPs with an average size of 2.85 nm are synthesized and uniformly dispersed in RP-3, exhibiting long-term stability with a sedimentation rate below 7% after 60 days. To evaluate the catalytic performance and reveal the complex catalytic cracking mechanism of hydrocarbon fuels under supercritical conditions, a combined approach of tubular reactor experiments and reactive force field molecular dynamics (ReaxFF MD) simulations is employed. Both experimental and simulation results demonstrate that, compared to thermal cracking, Pd/RP-3 catalytic cracking exhibits significant improvements in conversion, gas yield, olefin selectivity, and heat sink. At 700 °C, 200 ppm Pd NPs increase the heat sink of RP-3 from 2.52 MJ/kg to 2.77 MJ/kg. Kinetic analysis reveals that the enhancement is ascribed to the remarkable catalytic abilities of Pd NPs to reduce the activation energies for RP-3 cracking, C-C and C-H bond cleavage by approximately 66.7%, 80.7%, and 78.7%, respectively. Pd also enhances dehydrogenation reactions, leading to higher yields of hydrogen and olefins, while effectively facilitating benzene rings decomposition within the aromatic components of RP-3. The synthesized oil-dispersible Pd NPs present great potential for enhancing the cooling capacity and the catalytic cracking mechanism proposed here may provide a theoretical foundation for designing efficient future catalysts.
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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).
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Catalysts
·
2025
·Vol. 15
·期 2
·175
·
IF 4
Wei Wang,Jiaqi Liu,Guang Shi,Shiqi Wu,Shihan Zhang,Ruixia Yuan
A magnetic shell-structured nano-catalyst was prepared by self-polymerization of dopamine wrapped by ferric oxide as the carrier, which was loaded with palladium nanoparticles (Pd/PDA@Fe3O4). The presence of magnetic Fe3O4made it easy for nanoscale palladium particles to recover and prevent the loss of palladium nanoparticles that is unavoidable in traditional usage and preparation procedures. The catalyst was characterized by X-ray diffraction, fourier transform infrared spectroscopy, scanning electron microscopy, thermal weight loss analysis, Raman spectroscopy, X-ray photo-electron spectroscopy, and magnetic properties analysis. The catalytic performance of the prepared catalyst was investigated taking 4-nitrophenol (10 mg/L) and rhodamine B (15 mg/L) as the target pollutants. The results showed that under the conditions of 35 °C, pH = 7 and a catalyst dosage of 3 mg, the catalytic reduction efficiency of 4-nitrophenol, rhodamine B, and the mixture of them all can reach 99%. The catalytic efficiency of Pd/PDA@Fe3O4remained above 90% after being used 10 times. The shell structure of Fe3O4made it possible and easy to recover and recycle the nanoscale palladium, which was a real problem in the usage of nano-catalysts. At the same time, the problem of separation and recovery of palladium nano-catalyst is solved by magnetism, which provides research ideas for the recycling and utilization of nano-materials.
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Chem
·
2022
·
IF 25.832
Xiaoqian Wei,Shaojia Song,Weiwei Cai,Xin Luo,Lei Jiao,Qie Fang,Xiaosi Wang,Nannan Wu,Zhen Luo,Hengjia Wang,Zhihong Zhu,Jing Li,Lirong Zheng,Wenling Gu,Weiyu Song,Shaojun Guo,Chengzhou Zhu
The development of Fe single-atom catalysts is greatly impeded by their lower oxygen reduction reaction (ORR) performance in acid electrolytes when compared with Pt/C catalyst. Herein, we report an unprecedented ORR catalyst consisting of Pd nanoclusters (Pd NC ) and Fe single atoms (Fe–N–C/Pd NC ). Experimental investigations and theoretical calculations indicate that the enhanced ORR activity results from the Pd NC -induced spin-state transition of Fe(II) from low spin to intermediate spin, activating O–O bond through the side-on overlapping and achieving the pathway transition from associative to dissociative process. The over-binding of OH∗ can be facilely released to suppress the site-blocking effect and accelerate the removal of OH∗. In acid conditions, Fe–N–C/Pd NC exhibits excellent ORR performance with impressive half-wave potential (0.87 V), insignificant decay after 30,000 cycles, and a high maximum power density of 920 mW/cm 2 in fuel cell, superior to Pt/C catalyst. This work provides an efficient pathway to design non-Pt catalysts through the spin-regulation strategy.
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Cancer Communications
·
2025
·
IF 24.9
Fanglin Tian,Jian Huang,Weina Fan,Xin Li,Yuning Zhan,Kexin Zhu,Xiangyu Wang,Xin Hong,Xin Wang,Jin Ren,Ying Xing,Li Cai
Background Eps15 homology domain (EHD) proteins, including EHD1 to EHD4, play vital roles in tumor progression. In this study, we aimed to investigate which specific EHD proteins, if any, are implicated in tumor immune evasion and immunotherapy response. Methods The immunotherapy responses of lung adenocarcinoma (LUAD) patients were predicted using tumor immune dysfunction and exclusion (TIDE) analysis. The T cell killing assay was performed by co-culturing activated T cells with LUAD cells. The function of EHD1 as a regulator of programmed death-ligand 1 (PD-L1) endocytic recycling was determined by receptor internalization assays. Methylated RNA immunoprecipitation (MeRIP) was performed to investigate N6-methyladenosine (m 6 A) modification of EHD1 mRNA. The protein-protein interaction was revealed by the molecular docking analysis and validated by immunofluorescence (IF) and immunoprecipitation (IP) assays. RNA immunoprecipitation (RIP) was used to examine the interaction between YTH N6-methyladenosine RNA-binding protein 1 (YTHDF1) and EHD1 mRNA. The regulatory mechanism of YTHDF1 on EHD1 was investigated through the application of m 6 A-binding site mutation analysis. The murine LUAD cells were employed to establish subcutaneous xenograft models within immunocompetent C57BL/6 mice to assess the immunomodulatory impact of EHD1 in vivo. Results TIDE algorithms and survival analysis identified that EHD1 promoted LUAD immune escape. EHD1 knockdown enhanced T cell cytotoxicity in killing LUAD cells across all effector-to-target (E/T) ratios. EHD1 overexpression exerted the opposite effect. The molecular docking analysis revealed an interaction between EHD1 and the PD-L1 protein, verified by IF and IP. Furthermore, EHD1 knockdown inhibited PD-L1 recycling, thereby promoting its lysosomal degradation. Disruption of the EHD1/PD-L1 interaction impaired the regulatory function of EHD1 in tumor immune evasion. In an immune-competent mouse model, we found that EHD1 silencing impeded tumor immune evasion and enhanced the efficacy of anti‑PD‑1 therapy. MeRIP-qPCR confirmed obvious m 6 A modification of EHD1 . Further, the EHD1 mRNA was found to bind to the YTHDF1 protein, an m 6 A reader. YTHDF1 overexpression up-regulated EHD1 expression by enhancing its mRNA stability in an m 6 A-dependent manner. Conclusion Our study illuminates the role of m 6 A-modified EHD1 in tumor immune evasion and immunotherapy responses, thereby offering a novel avenue to potentially enhance immunotherapeutic sensitivity and improve the prognosis for patients with LUAD.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Decun Luo,Ziyu Tang,Xiyang Yu,Tao Zhang,Chun-Ran Chang,Zhun Hu
The effect of ZrO 2 crystalline phases on Pd/ZrO 2 for catalytic combustion of toluene was investigated. It was found that Pd/t-ZrO 2 showed superior activity when the toluene concentration was lower than 2000 ppm, while Pd/m-ZrO 2 performed better with toluene concentration higher than 3000 ppm. Kinetic studies showed that the reaction order of toluene on Pd/t-ZrO 2 and Pd/m-ZrO 2 is 0 and 2, respectively. The catalytic activity was controlled by combined effect of PdO activity and quantity, which was correlated with the interaction between palladium and zirconia. The t-ZrO 2 increased PdO species activity, while m-ZrO 2 could enhance the amount of PdO. DFT results showed that the p-band center of the O of PdO on t-ZrO 2 was higher, suggesting that PdO was more active. In situ -DRIFTS revealed that the reaction pathway of catalytic oxidation of toluene on Pd/ZrO 2 was as follows: toluene was oxidized stepwise to benzyl alcohol, benzaldehyde, benzoic acid , CO 2 and H 2 O.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Haoqiang Feng,Yike Li,Xian Liu,Kang Wang,Qianhao Du,Yingju Wang,Zhongjun Li
Developing efficient piezo-photocatalysts through integrating cation vacancies with double metal single atoms is vitally important for hydrogen production, while it remains a challenge. In this work, cadmium vacancy (V Cd ) as well as Pt and Pd single atoms (Pt-Pd) were simultaneously introduced into CdS to construct V Cd -CdS/Pt-Pd catalysts for piezo-photocatalytic hydrogen evolution. In-depth characterizations and DFT calculations confirmed that the symmetry breaking caused by V Cd , Pt-Pd dual single atoms and ultrasonic could induce the polarization enhancement and charge asymmetric distribution, modulate the density of electronic states as well as optimize the adsorption of H* intermediates. Under light and ultrasound, the optimal V Cd -CdS/Pt 0.20 -Pd 0.30 achieved the piezo-photocatalytic hydrogen evolution rate of 104.4 mmol g −1 h −1 , which was 10.0 and 30.7 times that of V Cd -CdS and CdS, respectively. The significant improvement of piezo-photocatalytic performance was due to the synergistic interaction of V Cd -CdS, Pt-Pd double single atoms and the ultrasonic-induced external stress, which enhanced the polarized electric field in V Cd -CdS/Pt-Pd and promoted the separation and transfer of photo-generated charges. Moreover, the piezoelectric polarization induced by ultrasonic could tilt the energy band and produce a stronger reduction potential, also facilitating the hydrogen evolution reaction. On the whole, the symmetry breaking achieved by structure modifications coupled with external stress effectively boosted the piezo-photocatalytic hydrogen evolution performance, which provided a reference for the design of high-efficiency piezo-photocatalysts based on vacancy engineering and double single atoms doping.
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ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Songyun Tao,Xiao Wang,Cheng Rao,Kaijie Liu,Yannan Li,Zhaoxu Yuan,Guan Peng,Yang Lou,Jun Ye,Hai Liu,Zeshu Zhang,Xiangguang Yang,Yibo Zhang,Shuyan Song
Enhancing catalytic performance through precise control of active site interactions still poses significant challenges. Diverging from conventional static methods, this study pioneers an innovative current-assisted approach to achieve precise, in situ dynamic tuning of electron transfer specifically within Pd-Ce diatomic sites. The groundbreaking current-assisted Pd 1 -Ce 1 /ATO catalyst achieves unprecedentedly low-temperature methane combustion performance, with a remarkable T 50 of 181 °C and a record-high turnover frequency (TOF 260 °C ) of 4.25 × 10 −2 s −1 . The current-induced augmentation of electron transfer from Ce to Pd markedly elevates the electron density around Pd centers , orchestrating dynamic modulation to synergistically enhance catalysis. This modulation amplifies the electron backdonation from electron-rich Pd to the methane C─H bond, facilitating efficient C─H bond scission, while promoting lattice oxygen mobility near Pd 1 -Ce 1 sites by tuning orbital energy matching, thus significantly amplifying the catalyst's oxidation capacity. The synergistic interplay of these electronically tuned factors promotes the formation of a four-center transition state (H 3 C δ − -Pd-O-H δ + ), effectively weakening the C─H bond and dramatically accelerating methane catalytic oxidation. This work not only achieves ultra-low-temperature catalytic activity with minimal noble metal loading but also establishes a paradigm shift in the rational design of advanced combustion catalysts, enabling on-demand modulation of catalytic activity through real-time regulation of inter-site interactions .
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CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Xing Yan,Dongren Cai,Meihong Lin,Zhijie Wu,Yegang Xia,Yanmei Cai,Sajid Ali,Kok Bing Tan,Andriambinintsoa Ranaivoson Tojonirina,Hao Sun,Guowu Zhan
The selective hydrogenation of CO 2 to methanol demands precise control of both catalyst architecture and reaction pathways. Here, we design an atomic layer deposition (ALD)-engineered Pd/ZnO/ZrO 2 ternary catalyst with atomic-scale ZnO interlayers to decouple and reconfigure active sites at dual interfaces (Pd-ZnO and ZnO-ZrO 2 ). This interfacial engineering drives a 7-fold enhancement in methanol space–time yield (0.584 vs. 0.084 g MeOH g cat −1 h −1 ) and switches the dominant reaction pathway from CO-mediated to formate-driven selectivity (methanol selectivity remarkably surges from 6 % to 64 %). Multimodal characterization and theoretical calculations reveal that ZnO interlayers orchestrate bifunctional cooperation: activating CO 2 /CO adsorption while suppressing CO/CH 4 formation through electronic effects. Long-term stability study uncovers a dynamic restructuring mechanism, where Pd-ZnO interfaces gradually evolve into PdZn β alloy phases under the reaction conditions. This work establishes ALD-mediated interface design as a generalizable strategy to manipulate reaction networks and methanol selectivity in catalytic CO 2 hydrogenation systems.
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