Catalysis Science & Technology
·
2026
·
IF 4
Ziheng Li,Junxin Guo,Haoze Liu,Dule Huhe,Zhao Wang
Despite their high methanol selectivity in CO2 hydrogenation, In2O3-based catalysts still face limitations in CO2 conversion and long-term stability. This work addresses these challenges by designing a highly dispersed Pd/In2O3 catalyst supported on self-pillared silicalite-1 (SP-S-1) zeolite. The well-defined channels and abundant surface silanol groups of SP-S-1 effectively anchor and disperse In2O3 nanoparticles. This structure also spatially isolates Pd species, which prevents their sintering and inhibits the formation of inactive Pd–In alloys. Comprehensive characterization reveals that the strong metal-support interaction stabilizes oxygen vacancies and prevents over-reduction of In3+ species, which are crucial for CO2 activation and methanol selectivity. The optimized Pd/In2O3/SP-S-1 catalyst achieves a methanol space-time yield of 2.57 gMeOH·gIn+Pd-1·h-1 at 300 °C, approximately five times higher than that of the unsupported counterpart. More importantly, it demonstrates high stability, retaining 95% of its initial activity after 100 hours on stream, far outperforming the unsupported catalyst. This work highlights zeolite confinement as a versatile strategy for designing robust and efficient CO2-to-methanol catalysts.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2026
·
IF 19.7
Zhiwen Li,Jiari He,Zaiqi Li,Jia Song,Difei Xiao,Haixia Liu,Yuanyuan Liu,Peng Wang,Zhaoke Zheng,Hefeng Cheng,Ying Dai,Baibiao Huang,Zeyan Wang
Pulsed electrocatalytic CO 2 reduction reaction (p-CO 2 RR) on copper-based catalysts can dynamically stabilize active Cu + sites and enrich surface *OH, enabling sustained CO 2 -to-C 2+ conversion. However, its practical application is still constrained by: 1) low time efficiency caused by both the inherent instability of Cu + during cathodic polarization and the sluggish re-oxidation of Cu 0 to Cu + , and 2) inadequate CO 2 -to-C 2+ conversion efficiency caused by the insufficient *OH coverage. To address these challenges, a Pd-modified Cu 2 O catalyst (Pd-Cu 2 O) with strong Pd-Cu electron interaction is designed. In situ experiments and theoretical studies reveal that Pd induces stable electron-deficient Cu + /Cu 0 sites, which effectively suppressing Cu + reduction during the cathodic phase and promoting Cu + regeneration during anodic phase, thus shortening the required oxidation duration. Concurrently, Pd accelerates water dissociation and enhances *OH coverage, which facilitates *CO adsorption and enhances C-C coupling. As a result, Pd-Cu 2 O achieves a Faradaic efficiency for C 2+ of 79.8 % with stable operation for over 50 h, and the time efficiency exceeding 87 %, outperforming most reported p-CO 2 RR catalysts. This work highlights the importance of rational catalyst design via electronic structure regulation for enhancing the time efficiency and C 2+ production performance for p-CO 2 RR, paving the way for efficient CO 2 -to-C 2+ conversion and practical applications.
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Materials Today Energy
·
2026
·
IF 8.6
Yakai Hao,Mingqiu Bao,Huijin Chen,Yuchuan Zhu,Ruoxi Yang,Ruirui Yue,Jinbing Shu,Jingkun Xu
Catalysts with high-efficient performance, high durability and low cost are still urgently needed to promote the wide application of direct alcohol fuel cells (DAFCs). This work prepared a PdNi/PPy composite by dispersing Ni-doped Pd nanoparticles on coarse polypyrrole (PPy) granules via facile interfacial redox and polymerization. The optimized PdNi/PPy composite possesses a porous morphology and uniform dispersion, which are key for achieving performance synergistic optimization in alcohol oxidation reactions (AORs). Specifically, for ethylene glycol oxidation (EGOR), the PdNi/PPy achieves mass activity (MA, 5577.2 mA mg Pd −1 ), specific activity (SA, 32.3 mA cm −2 ), and intrinsic activity (TOF, 6.8 s −1 ), which are 7.9, 3.0 and 2.7 times those of commercial Pd/C, respectively. It also exhibits higher activity for ethanol and methanol oxidation compared to other catalysts. Characterizations demonstrate that the synergy between Ni-doped Pd and conductive PPy significantly enhances catalytic properties. The electronic structure of Pd is optimized via Ni-doping induced d-band center modulation and efficient interfacial charge transfer through heterojunction formation. Additionally, the PPy support facilitates uniform dispersion and maximizes active site exposure. This work can offer meaningful insights for the development of advanced anode catalysts by effective doping of active metals and further strengthening of the carrier effects for DAFCs.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 13.2
Wenxing Jiang,Yuanting Peng,Qiqi Wan,Endao Zhang,Junbo Hou,Xiaodong Zhuang,Changchun Ke
Direct ammonia borane fuel cells (DABFCs) offer promising portable energy solutions but face limitations from sluggish anodic kinetics and electrode degradation. This study introduces a three-dimensional hierarchical Pd-integrated nanostructured electrode (Pd-INE) synergizing nanostructuring with interfacial engineering. Vertically oriented Pd-decorated nanosheets are electronically coupled to nickel foam (NF) via Ni(OH) 2 , maximizing active site accessibility and structural stability. Density functional theory (DFT) confirms 1.18 e − transfer from Pd to Ni(OH) 2 generates electron-deficient Pd sites that weaken NH 3 BH 3 adsorption (ΔE ads = −0.92 eV) while enabling bifunctional catalysis: Pd activates B H bonds and Ni(OH) 2 -derived interfacial hydroxyls drive B O formation. Pd-INE demonstrates superior ammonia borane oxidation activity versus conventional polymer-bound Pd/NF while achieving a record peak power density of 724.1 mW cm −2 at 80 °C in DABFC operation, 2.3 times higher than both Pd/NF (321.2 mW cm −2 ) and prior benchmarks (315 mW cm −2 ). This enhancement stems from vertical nanosheets enhancing mass/charge transport and DFT-validated electronic interactions optimizing intermediate adsorption energies. The anode exhibits exceptional durability with 35 μV h −1 voltage decay over 40 h, outperforming polymer-bound anodes by 150-fold. This work establishes an ionomer-free anode paradigm resolving activity-durability trade-offs in direct liquid fuel cells through atomically tailored bifunctional interfaces.
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ChemCatChem
·
2019
·Vol. 11
·期 20
·5098-5107
·
IF 4.495
Ning Xiang,Yaqin Hou,Xiaojin Han,Yulin Li,Yaoping Guo,Yongjin Liu,Zhanggen Huang
Room temperature HCHO catalytic oxidation over inert support loaded Pd catalysts remains a significant challenge. Herein, a series of alkali Na (1–4 wt.%) modified 1Pd/SBA-15 catalysts were prepared by a co-impregnation method and used for HCHO catalytic oxidation at room temperature. Results showed that alkali Na significantly improved the HCHO oxidation performance of 1Pd/SBA-15 and the optimal Na loading was 2 wt.%. BET, XRD, STEM, XPS, H 2 -TPR, O 2 -TPD and in situ DRIFTS were performed to reveal the promotion role of alkali Na. As a consequence, alkali Na addition could stabilize well dispersed Pd particles which then facilitated the O 2 activation and accelerated the decomposition of formate intermediates species, thus a superior HCHO catalytic oxidation performance was obtained. This study first clearly illustrated the promotion mechanism of alkali Na without the implication of active support and provides an efficient and facile way to achieve high dispersion of Pd particles on inert support and tremendously expands the selected range of supports for room temperature HCHO catalytic oxidation. Graphical Alkali promoted : A series of Na alkali-promoted 1Pd/SBA15 catalysts were prepared by a co-impregnation method and tested for HCHO catalytic oxidation at room temperature. Addition of alkali Na stabilized well-dispersed Pd particles which facilitated O 2 activation and accelerated formate species decomposition rate, leading to superior HCHO catalytic oxidation performance of 2Na-1Pd/SBA-15.
研究领域:
催化化学
·
环境科学
·
材料化学
·
表面科学
·
大气污染控制
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高影响因子
CATALYSIS COMMUNICATIONS
·
2016
·
IF 3.389
Wenhuan Dong,Saisai Cheng,Cheng Feng,Ningzhao Shang,Shutao Gao,Chun Wang
Well-dispersed and ultrafine metal nanoparticles can significantly improve the catalytic performance of heterogeneous catalyst. In this paper, highly dispersed Pd nanoparticles were successful anchored on reduced graphene oxide using a co-deposition and sacrificial method, in which cobalt was used as the sacrificial agent. This method can effectively prevent the Pd nanoparticles from aggregation, and the resulted catalyst exhibited exceedingly high catalytic activity for the reduction of 4-nitrophenol at room temperature with NaBH 4 as hydrogen resource. The turnover frequency reaches 9900 h − 1 at 298 K, which is among the highest values ever reported thus far for heterogeneously catalyzed reduction of 4-nitrophenol under ambient conditions.
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Science China-Materials
·
2018
·Vol. 62
·期 3
·351-358
·
IF 4.318
Tang Yonghua,Zhou Peng,Chao Yuguang,Lin Fei,Lai Jianping,Li Hongxing,Guo Shaojun
Photocatalytic hydrogen production represents a promising strategy for clean, sustainable, and environmentfriendly energy supply. Up to now, great efforts have been devoted to designing the photocatalysts with noble metal as co-catalyst for visible-light-driven hydrogen evolution, while more efficient photocatalytic systems are still a major challenge. Herein, we report a facile strategy for synthesizing face-to-face ultrathin Pd nanosheets-amorphous carbon nitride (Pd NSs-ACN) structure with large contacting interface and short electronic transmission pathway, which can work as an efficient photocatalyst for hydrogen production. The synthesis starts with the growth of ultrathin Pd NSs, followed by assembly with the visible-light-response ACN through a simple stirring and annealing procedure. The resultant two dimensional face-to-face structures deliver an average hydrogen generation rate of 1.45 mmol h −1 g −1 at a temperature of 25°C, almost 2.6 times higher than that of Pd Nps-ACN with particle- to-face structural feature. The efficient photocatalytic activity is ascribed to the formation of high-density of active sites between ultrafine face-to-face contacted Pd NSs and the ACN, which cooperate more synergistically towards photocatalytic hydrogen production. The face-to-face engineered Pd NSs-ACN hybrids also offer a good stability revealed by photocatalytic hydrogen production measurements. The extraordinary performance highlights a powerful engineering model for designing other face-to-face contacting co-catalyst/photocatalysts, which will be a great impetus to optimize new catalytic transformations.
研究领域:
材料科学
·
光催化
·
纳米技术
·
氢能
·
可持续能源
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高影响因子
CHEMPHYSCHEM
·
2015
·Vol. 16
·期 18
·3865-3870
·
IF 3.419
Baohua Zhang,Yiguo Xue,Zhimin Xue,Zhonghao Li,Jingcheng Hao
The ionic liquid 1-ethyl-3-methylimidazolium acetate ([EMIM]Ac) is investigated as a solvent for the synthesis of Pd particles. Interestingly, nanosheet-constructed Pd particles could be successfully synthesized in [EMIM]Ac without any additional reducing agent and template under ionothermal conditions. [EMIM]Ac itself works as the solvent, the reducing agent, and the template for the formation of these interesting Pd particles, making this method complementary to the well-known ionic-liquid-precursor approach. Furthermore, [EMIM]Ac can be recycled with no loss of activity for the formation of nanosheet-constructed Pd particles within our studied cycles. Specifically, the nanosheet-constructed Pd particles exhibit superior electrocatalytic activity and stability towards ethanol oxidation and formic acid oxidation compared with commercially available Pd black catalyst, thus demonstrating their promising applications in fuel-cell area. The current approach, thus, presents a green approach towards the synthesis of Pd particles, using only a simple palladium salt and an ionic liquid. Graphical A neat synthesis : A facile green route is proposed for the synthesis of nanosheet-constructed Pd particles in an ionic-liquid solvent without any additional reducing agent and template for efficient electrocatalytic applications.
研究领域:
材料科学
·
纳米技术
·
电化学
·
绿色化学
·
催化
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ELECTROANALYSIS
·
2024
·Vol. 36
·期 10
·e202400028
·
IF 2.7
Suning Man,Junying Zheng,Yi Zhang,Lei Huang,Xiaoping Wu
Given the high solubility and mobility of hexavalent chromium in the environment and edible plants, the development of a suitable method for the screening and quantification of Cr(VI) is highly desirable. Herein, a selective and sensitive sensing method for detecting Cr(VI) in food grains was established, using an electrodeposited gold-palladium bimetallic nanoparticles (BNPs) based electrochemical sensor and a microwave digestion procedure for chromium dissolution. The sensor interface was characterized by scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX) and cyclic voltammetry. The results indicate that the fabricated sensor has a larger active surface area and an enhanced electrocatalytic effect compared to the monometallic modification, leading to a significant increase in the electrochemical reduction current of Cr(VI) as a consequence of synergistic effects. Using square wave anodic stripping voltammetry, the sensor demonstrates a wide linear range (5–3000 μg L −1 ) and a low detection limit of 2.7 μg L −1 for Cr(VI), as well as considerable repeatability and stability. Satisfactory selectivity towards Cr(VI) was also demonstrated, even in the presence of 500-fold Cr(III) and 100-fold common heavy metal ions like Cd(II), Pb(II), and Hg(II). The proposed sensing method offers a promising alternative for rapidly identifying toxic Cr(VI) in water and food grains.
研究领域:
环境监测
·
食品安全
·
电分析化学
·
纳米材料
·
传感器与生物传感器
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Ziqiang Wang,Zechuan Dai,Hongjie Yu,Hugang Zhang,Wenjing Tian,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Electrochemical ammonia synthesis is considered as an alternative sustainable method to the traditional Haber–Bosch process because of the reduced energy consumption and mild operation conditions. The key is to design efficient electrocatalysts for facile adsorption and activation of nitrogen. Herein, a nanoporous Pd film with a tunable pore size has been in situ grown on Ni foam (nPd/NF) via a micelle-assisted replacement method using NF as a reductant and substrate, where polystyrene-b-poly(ethylene oxide) and 1,3,5-triisopropylbenzene serve as a pore-forming agent and a swelling agent, respectively. Combining the continuous large nanoporous structure and self-supported properties, the obtained nPd/NF exhibits excellent catalytic performance for ammonia synthesis with a high NH3 yield of 18.27 μg h–1 mgcat–1 and a faradaic efficiency of 10.36% in 0.1 M Na2SO4. This work provides a fascinating route for the rational design of self-supported porous noble metals with a tunable pore size for effective electrosynthesis of ammonia.
研究领域:
材料科学
·
电化学
·
催化化学
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International Journal of Electrochemical Science
·
2023
·
IF 1.5
Qizhi Dong,Tianwu Yin,Hansheng Wan,Guiming Zhu,Gang Yu,Cancheng Guo
Based on electrostatic self-assembly technology, Pd electrocatalyst with high efficiency and excellent CO-tolerance, which is supported on TiO 2 surface modified by amino-rich, cationic poly (diallyldimethylammonium chloride) (PDDA), was prepared. Through electrostatic interaction, Pd precursors were uniformly distributed on TiO 2 (P) and then in situ reduced into Pd nanoparticles (NPs). in such process, PDDA produced a large number of amine to facilitate the uniform distribution of Pd NPs on the surface of TiO 2 . After that，Pd/TiO 2 (P) was mixed with carbon black as anodic catalysts for formic acid oxidation reaction. Transmission electron microscope images and X-ray diffraction patterns revealed that Pd NPs with an average size of ∼3 nm were uniformly dispersed on TiO 2 . Moreover, with the application of cyclovoltammetry and chronoamperometry, we demonstrated the significant enhancement in the electrocatalytic activity and the tolerance toward CO poisoning when compared with Pd/TiO 2 -C for direct formic acid fuel cells.
研究领域:
材料科学
·
电化学
·
能源科学
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高影响因子
ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Shaoda Huang,Shuanglong Lu,Hongyin Hu,Binbin Cao,Huining Li,Fang Duan,Han Zhu,Hongwei Gu,Mingliang Du
Palladium-based catalyst represents one of the most promising candidates among all non-platinum oxygen reduction reaction (ORR) catalysts. However, it is still challenging to precisely engineering their morphology and composition . Herein, highly branched core-shell PdCu@Pd nanocrystals have been fabricated via a simple one-pot synthesis that co-directed by hydrogen gas and halide ions. Such unique PdCu@Pd nanocrystals exhibit prominent ORR activity, durability and methanol-tolerance in alkaline media owing to their core-shell composition , highly-branched structure and defect-rich surface. This work elucidates a facile strategy to design highly branched core-shell nanomaterials , shedding light on the exploration and optimization of novel non-platinum ORR catalysts.
研究领域:
材料科学
·
电化学
·
催化科学
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高影响因子
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