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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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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高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Yi Wu,Xinyu Dai,Jun Yu,Zhongxin Song,Lei Zhang
Proton-exchange membrane fuel cells (PEMFCs) constitute an advanced clean technology that efficiently transforms hydrogen energy into electricity. However, the hydrogen oxidation reaction (HOR) at the anode heavily depends on precious metal catalysts, posing economic challenges for PEMFCs commercialization. Consequently, developing cost-effective, high-activity HOR catalysts for anodes is imperative. In this study, we developed a bimetallic Pd–Pt electrocatalyst for acidic HOR, enhancing the catalytic activity by modulating the electron transfer between the metals. X-ray photoelectron spectroscopy and X-ray absorption near-edge spectroscopy confirmed the presence of negatively charged Pt atoms. Electrochemical tests showed that PdPt0.1 exhibited exceptional catalytic activity, with mass activities 3.2 and 11.5 times higher than those of commercial Pt/C and Pd/C, respectively. Moreover, in membrane electrode assembly tests, PdPt0.1 achieved a power density of 1.19 W cm–2, outperforming commercial Pt/C with a power density of 0.85 W cm–2. These remarkable performances are attributed to electron transfer between Pd and Pt, reducing the hydrogen binding energy during HOR. This study offers valuable insights for the controlled design of HOR catalysts based on the electron-transfer direction.
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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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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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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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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Hongxia Liu,Meng Wang,Xuqiang Zhang,Jiantai Ma,Gongxuan Lu
The development of an active but cheaper catalyst is critical for efficient photocatalytic hydrogen from renewable source. In this study, we develop a high active catalyst for hydrogen evolution from formaldehyde via alloying of Pd with Ag and sensitization with a dye eosin Y (EY). The XRD, XPS, TEM and HRTEM characterizations indicate that the catalyst exhibits a core-shell structure (Ag core and Ag-Pd shell). Alloying Pd with Ag not only provides more efficient catalytic sites than single component Pd catalyst, but greatly promotes the efficient electron transfer and prolongs the lifetime of photogenerated electrons, enhances the charge separation efficiency and the photocatalytic hydrogen evolution activity significantly. The catalyst activity for hydrogen is highly dependent on the adsorption energies of HCHO and H 2 O molecules on metal surface of the alloy catalyst. Our results disclose a new route to high efficient catalyst development for solar hydrogen generation from formaldehyde.
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高影响因子
Analytical Methods
·
2018
·Vol. 10
·期 15
·1703-1708
·
IF 2.073
Jiao Ma,Chengcheng Yang,Shu Zhu,Jinyi Song,Yingzi Fu
In this paper, a simple stereoselective sensing platform for the recognition of ascorbic acid (AA) and isoascorbic acid (IAA) was fabricated via immobilizing HS-β-cyclodextrin (HS-β-CD) on the surface of nanocomposite modified glassy carbon electrodes (GCEs). The nanocomposites were prepared using Pt and Pd bimetal nanowires (Pt–PdNWs) and reduced graphene oxide (rGO). The preparation process was characterized by scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), cyclic voltammetry (CV) and differential pulse voltammetry (DPV). After the modified electrodes interacted with the analytes, obvious differences in the peak currents of AA and IAA were obtained, hinting at the ability of the proposed sensor to recognize AA and IAA. This sensor with simple preparation, a rapid response, and excellent stability and reproducibility provided a promising perspective to recognize and determine AA and IAA.
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高影响因子
ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Jixuan Han,Shimeng He,Xinyue Liu,Ziyi Gao,Jiayu Xiao,Yuanhong Sun,Xiaocui Fang,Lilusi Ma,Chen Wang,Xuzhen Qin,Yanlian Yang
Lung cancer is a leading cause of cancer mortality, yet early diagnosis remains difficult, highlighting the need for sensitive, noninvasive methods. Extracellular vesicles (EVs) and their surface proteins (e.g., PD-L1) are promising biomarkers; nevertheless, current EV detection requires time-consuming purification, sophisticated instrumentation, and long measurement protocols, resulting in high expenses and operational difficulties. This study developed an integrated colorimetric sensor, IMAN, based on a strategy of “Immunomagnetic Microbeads (IM) capture + Aptamer(Apt) recognition + Nanozyme (N) catalysis”. IMAN employs magnetic beads modified with antibodies against CD9 and CD81 to directly capture EVs from serum, eliminating the need for time-consuming prior isolation; combined with a one-step colorimetric readout, the entire workflow can be completed with only ∼40 min of hands-on time, requiring no complex instrumentation. The PD-L1 protein on the EV surface is specifically recognized by a nanoparticle-bound nucleic acid aptamer. Signal generation is achieved through the catalytic oxidation of 3,3',5,5'-tetramethylbenzidine (TMB) by a platinum-gold bimetallic nanozyme (Pt@Au). The facile IMAN colorimetric method demonstrated a relatively broad dynamic range (107–1010 particles/mL), high specificity (unaffected by 100 pg/mL soluble PD-L1 in serum), and reproducibility (relative standard deviation, RSD = 9.1%). Analysis of clinical serum samples revealed significantly elevated EV-PD-L1 levels in patients with lung cancer compared with healthy donors and patients with benign nodule (p < 0.01). Receiver operating characteristic (ROC) analysis yielded areas under the curve (AUC) of 0.849 for distinguishing patients with lung cancer from healthy donors and 0.860 for distinguishing patients with lung cancer from patients with benign nodules, which are superior to those of the conventional serum biomarkers CEA and Cyfra21-1. By addressing the cost, complexity, and slow response of current methods, IMAN offers a simple, cost-effective platform for direct EV surface protein detection without complex instrumentation, providing a novel tool for the noninvasive lung cancer diagnosis.
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高影响因子
ELECTROCHIMICA ACTA
·
2014
·
IF 4.086
Qian-Li Zhang,Jie-Ning Zheng,Tian-Qi Xu,Ai-Jun Wang,Jie Wei,Jian-Rong Chen,Jiu-Ju Feng
A simple, facile, and one-pot solvothermal strategy was developed to prepare Pd-on-Cu nanoparticles evenly distributed on reduced graphene oxide (Pd-on-Cu/RGO) in ethylene glycol systems, using cetyltrimethylammonium bromide (CTAB) as a structure-directing agent. Control experiments were demonstrated the critical role of CTAB and GO to the final morphology. The as-prepared nanocomposites exhibited the enlarged surface area of 64.98 m 2 g −1 Pd, improved electrocatalytic activity, and better stability for ethanol oxidation in alkaline media, which can serve as promising anode catalysts in direct alcohol fuel cells.
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Nano Research
·
2015
·Vol. 8
·期 6
·2115-2123
·
IF 7.01
Long Ran,Wu Di,Li Yaping,Bai Yu,Wang Chengming,Song Li,Xiong Yujie
Heterogeneous catalysis occurs through a process of interfacial reactions; therefore, both surface facet and size control can increase catalytic efficiency. Octahedral Pd nanocrystals, enclosed by {111} facets, should be the ideal geometrical shape for Heck coupling reactions; however, it is challenging to synthesize 5 nm Pd octahedrons with a relatively uniform size distribution using existing capping-agent techniques. Here, we used palladium as a model system to investigate how the kinetics of atomic addition could be precisely controlled using a syringe pump. As a result, our method produced Pd octahedrons as small as 5 nm, which increased the catalytic efficiency of Heck coupling reactions while reducing the weight of catalyst used.
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