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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2022 · IF 7.139

Pd/In2O3-based bilayer H2 sensor with high resistance to silicone toxicity and ultra-fast response

Wenxin Liu,Jiabin Zou,Shuni Li,Jinkun Li,Feihu Li,Zili Zhan,Yeguang Zhang

Hydrogen sensors are easily deactivated by hexamethyldisiloxane (HMDSO) poisoning. Moreover, the existing anti-poisoning strategies can also damage the overall sensing performance of these hydrogen sensors. Therefore, a new bilayer design with a Pd/In 2 O 3 sensitive layer and an In 2 O 3 /Al 2 O 3 catalytic filter layer is proposed to avoid the deactivation of hydrogen sensors. The In 2 O 3 /Al 2 O 3 layer helps in hindering HMDSO and its decomposition products from reaching the Pd/In 2 O 3 layer. The H 2 response of the sensors is enhanced due to the small size of In 2 O 3 and the electronic sensitization of Pd. As a result, the bilayer sensors exhibit high response (Ra/Rg = 53) and ultra-fast response time (1 s) towards 3000 ppm H 2 at 365 °C. The resistance and the H 2 response of the bilayer sensors are almost unchanged after 40 min of 10 ppm HDMSO poisoning. In this paper, the mechanism of resistance against silicone poisoning and the H 2 response of the bilayer sensors are discussed from the separation of sensing and catalytic filtration reactions to the behavior of adsorbed oxygen.

研究领域: 材料科学 · 传感器技术
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Nanoscale · 2015 ·Vol. 7 ·期 17 ·7615-7623 · IF 7.394

In situ fabrication of a perfect Pd/ZnO@ZIF-8 core–shell microsphere as an efficient catalyst by a ZnO support-induced ZIF-8 growth strategy

Lu Lin,Tong Zhang,Haiou Liu,Jieshan Qiu,Xiongfu Zhang

Controllable encapsulation of nanoparticles with metal organic frameworks (MOFs) has been an efficient way to impart the unique chemical and physical properties of the nanoparticles to metal organic frameworks and create new types of multifunctional MOF core–shell materials with enhanced properties. Here, a novel ZnO support-induced encapsulation strategy is reported to efficiently fabricate a Pd/ZnO@ZIF-8 core–shell catalyst, with Pd/ZnO as the core and ZIF-8 as the shell. The novel synthesis procedure involves first loading Pd nanoparticles onto the surface of the ZnO microsphere to form a Pd/ZnO core and then coating the core with a layer of defect-free ZIF-8 shell via ZnO-induced in situ ZIF-8 growth to obtain the Pd/ZnO@ZIF-8 core–shell catalyst. It was crucial that the ZIF-8 was in situ formed from the ZnO core in an ethanol solution only containing 2-methylimidazole under mild conditions. This strategy allowed for the growth of ZIF-8 right on the surface of Pd/ZnO via the reaction between ZnO and the 2-methylimidazole ligands, and thus avoided the random deposition of ZIF-8 crystals on the Pd/ZnO core as in the case of the conventional ZIF-8 synthesis solution. Furthermore, use of ethanol as the solvent also favored achievement of the well-defined Pd/ZnO@ZIF-8 structure, since the ethanol solution of 2-methylimidazole was able to keep the balance between ZnO dissolution and ZIF-8 formation. The as-prepared Pd/ZnO@ZIF-8 core–shell microsphere as an efficient catalyst displayed excellent performance in terms of size-selectivity, stability and anti-poisoning in the liquid hydrogenations of alkenes.

研究领域: 材料科学 · 催化化学
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ELECTROCHIMICA ACTA · 2025 · IF 5.6

Pre-embedded strategy for anti-NOM poisoning performance of palladium nanoparticles in electrocatalytic dechlorination

Linpiao Cheng,Shuyue Liu,Yinan Liu,Xiangyi Tang,Mue Tang,Xinhua Xu,Xiaoshu Lv

Electrocatalytic hydrodechlorination (EHDC) represents a sustainable approach to detoxifying the chlorinated organic pollutants (COPs). However, electrodes often suffer from fouling due to the ubiquitous natural organic matters (NOM) in surface water bodies. Herein we demonstrated that pre-mixing humic acid (HA) with palladium nanoparticles (Pd NPs) is an ingenious approach to address this issue. The introduction of HA improved dispersion of Pd NPs, enhanced surface hydrophilicity to promote H* generation, and increased electrostatic repulsion and steric-hinerance against NOM in solution. As a result, the as-synthesized HA 0.2 -Pd electrode exhibits significantly improved EHDC performance and anti-NOM poisoning ability. In the batch experiment, the HA 0.2 -Pd NPs achieved removal efficiencies of 91.3 and 80.8 % respectively, for treating 50.0 mg L −1 of 2,4-dichlorophenol (2,4-DCP, a probe COP) from contaminated water in the absence or presence of 20 mg L −1 HA (representative of NOM) at -0.85 V vs . Ag/AgCl. Compared to that, the pure Pd/C electrode experienced a marked efficacy decline from 82.9 to 56.5 % in the presence of HA. Moreover, the HA 0.2 -Pd/C electrode maintained a steady efficiency above 92.0 % over 12 h EHDC in a continuous-flow cell, while only 60.0 % for the Pd/C electrode. When subjected to contaminated natural water, the HA 0.2 -Pd/C electrode afforded an EHDC efficiency of 75.4 %, significantly surpassing the 39.4 % efficiency of Pd/C electrode.

研究领域: 环境科学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Bidirectional controlling synthesis of branched PdCu nanoalloys for efficient and robust formic acid oxidation electrocatalysis

Bo Yang,Wanqing Zhang,Shenglan Hu,Chengzhou Liu,Xiaoqu Wang,Youjun Fan,Zhe Jiang,Jun Yang,Wei Chen

Through a two-way control of hexadecyl trimethyl ammonium bromide (CTAB) and hydrochloric acid (HCl), the PdCu nanoalloys with branched structures are synthesized in one step by hydrothermal reduction and used as electrocatalysts for formic acid oxidation reaction (FAOR). In this two-way control strategy, the CTAB is used as a structure-oriented surfactant , while a certain amount of HCl is used to control the reaction kinetics for achieving gradual growth of multi-dendritic structures. The characterizations including scanning transmission electron microscope (STEM), X-ray powder diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) suggest that PdCu nanoalloys with unique multi-dendritic branches have favorable electronic structure and lattice strain for electrocatalyzing the oxidation of formic acid. In specific, among the electrocatalysts with different Pd/Cu ratios, the Pd 1 Cu 1 branched nanoalloys have the largest electrochemically active surface area (ECSA) and the best performance for the FAOR. The catalytic activity of the Pd 1 Cu 1 branched nanoalloys is 2.4 times that of commercial Pd black. After the chronoamperometry test, the Pd 1 Cu 1 branched nanoalloys still maintain their original morphologies and higher current density than that of the commercial Pd black. In addition, in the CO-stripping tests, the initial oxidation potential and the oxidation peak potential of the PdCu branched nanoalloys for CO adsorption are lower than those of commercial Pd balck, evincing their better anti-poisoning performance.

研究领域: 材料科学 · 电化学
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ELECTROCHIMICA ACTA · 2021 · IF 6.901

The ethanol oxidation reaction on bimetallic PdxAg1-x nanosheets in alkaline media and their mechanism study

Xianzhuo Lao,Min Yang,Jianyu Chen,Lian Ying Zhang,Peizhi Guo

The direct ethanol fuel cells (DEFCs) are considered as a kind of green and sustainable portable power source with high energy density, stable convert efficiency and zero/low emissions. In this study, the Pd x Ag 1-x nanosheet assemblies (NSAs) composed of a 2D sheet structure are synthesized by a facile one-step method. Alloyed Pd x Ag 1-x NSAs perform better catalytic activities and anti-toxicity than that of pure Pd NSA, closely related to their macroscopic morphological characteristics and microscopic electronic structure. Also, the mechanisms of the common four electrons pathway of ethanol oxidation reaction (EOR) on Pd x Ag 1-x NSAs are studied using the cyclic voltammetry method. Higher catalytic temperature and concentrations of both the KOH and ethanol have a positive effect on the overall reaction of the EOR, especially for the rate determination step in anodic scanning and the removal of the oxygen containing Pd-related intermediate species during cathodic scanning. However, excessive concentrations of KOH and ethanol should be avoided due to the formation of the oxide layer embedded at the surface of Pd at higher potentials and the decrease in conductivity, respectively. So, appropriate reaction temperature and medium conditions are favorable for the catalytic reaction.

CAS / MDL: 1310-58-3
研究领域: 材料科学 · 电化学 · 能源研究
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NANO · 2017 · IF 1.025

One-Pot Synthesis of Nanodendritic PtIr Alloy with High Electrochemical Activity for Ethylene Glycol Oxidation

Xuedong Gao,Lulu Liu,Qiyu Wang,Kun Qi,Zhao Jin,Weitao Zheng,Xiaoqiang Cui

Nanodendritic Pt-based bimetallic alloys are one promising catalyst with three-dimensional (3D) networks structure composed of integrating branches for electrochemical catalytic reaction. We successfully synthesized dendrites Pt 6 Ir 4 alloy with small size of 20 nm in oleylamine. The dendritic Pt 6 Ir 4 alloy are characterized by high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The electrochemical tests suggest that the as-prepared dendritic Pt 6 Ir 4 alloy exhibits greatly enhanced ethylene glycol oxidation reaction (EGOR) activity than commercial Pt/C with high EGOR mass activity, anti-poisoning and stability.

研究领域: 材料科学 · 电化学
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Science China-Chemistry · 2022 ·Vol. 65 ·期 6 ·1112-1121 · IF 10.138

Two-dimensional PtPb-PbS heterostructure enables improved kinetics and highlighted bifunctional antipoisoning for methanol electrooxidation

Liu Liangbin,Tang Chongyang,Bu Lingzheng,Xiao Xiangheng,Huang Xiaoqing

Two-dimensional (2D) platinum (Pt)-based nanomaterials are considered as the ideal fuel cell catalysts, while their rational synthesis associated with phase control remains a formidable challenge. Herein, we firstly design the novel 2D Pt-lead-sulphur heterophased nanosheets (PtPbS HPNSs) as efficient high-toleration electrocatalysts for methanol oxidation reaction (MOR). They exhibit much higher activity and more highlighted bifunctional antipoisoning abilities than PtPb NSs and commercial Pt/C. Further density functional theory (DFT) simulation verifies that the decreased electron density of Pt sites worked by Pb and S makes CO intermediate favorable to desorb, avoiding the formation of CO*-polluted Pt sites. Simultaneously, this heterophased interface effectively weakens the adsorption of S 2− -species and improves the S-poisoning tolerance, showing a route to realize nearly innoxious catalysis. The present work highlights the importance of heterophase control in tuning antipoisoning property for 2D Pt-based nanomaterials, which is key for the rational design of efficient fuel cell anodic catalysts.

CAS / MDL: 112-55-0 112-90-3
研究领域: 材料科學 · 電化學 · 催化劑設計
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CATALYSIS COMMUNICATIONS · 2023 · IF 3.7

Construction of Pt decorated CeO2 nanocomposite for efficient VOCs catalytic oxidation and atmospheric total organic carbon dictation

Siyue Zhou,Jingjing Fang,Kai Chao,Liang Li

Toluene, dichloromethane, and methanethiol were selected as probe molecules for aromatic, chlorinated, and sulfurated VOCs, respectively, to evaluate the catalytic properties of Pt/CeO 2 composites. The T 90 for toluene, DCM, and methanethiol oxidation were only 153, 265, and 240 °C, when 0.9 wt% Pt/CeO 2 was used as the catalyst. The synergy between Pt and support could be responsible for the high catalytic activity and antipoisoning properties. When combined with NDIR CO 2 sensors, the composite could be used for atmospheric total organic carbon detection. The recorded data almost overlap with that of the theoretical, suggesting the excellent reliability of the dictation system.

研究领域: 环境科学 · 催化材料
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ACS Omega · 2018 · IF 0

Pt Nanoparticles Loaded on W18O49 Nanocables–rGO Nanocomposite as a Highly Active and Durable Catalyst for Methanol Electro-Oxidation

Yizhi Wang,Shuo Wang,Fan Li,Yan Wang,Huairuo Zhang,Chunwen Sun

Highly active and durable electrocatalysts are vital for commercialization of direct methanol fuel cells. In this work, a three-dimensional nanocomposite consisting of platinum nanoparticles, W18O49 nanocables, and reduced graphene oxide composite (Pt/W18O49 NCs–rGO) has been prepared as an electrocatalyst for methanol oxidation reaction (MOR). The catalyst is prepared through a two-step method. The W18O49 nanocables and the reduced graphene oxide composite are prepared by a solvothermal process. Then, Pt nanoparticles are loaded on the W18O49 nanocables and the reduced graphene oxide composite by a hydrogen reduction at ambient condition. The obtained catalyst has a special three-dimensional architecture consisting of two-dimensional nanosheets, assembled one-dimensional nanocables, and the loaded nanoparticles on their surface. The Pt/W18O49 NCs–rGO catalyst shows 1.56 time mass activities than the Pt/C, with the current density of the forward anodic peak reaching 1624 mA/mgPt at 0.854 V versus reversible hydrogen electrode potential in 0.1 M HClO4 and 0.5 M CH3OH mixed electrolyte. It also shows a strong antipoisoning property toward CO. For the durability testing, the current density of Pt/W18O49 NCs–rGO shows a 37% decay, whereas the current of Pt/C catalyst shows a 41% degradation from 600 to 3600 s at 0.7 V. The high activity toward MOR, good antipoisoning for intermediate products, and excellent stability are ascribed to strong metal–support interaction effects between the Pt nanoparticles and the W18O49 NCs.

CAS / MDL: 10025-99-7 13283-01-7
研究领域: 材料科学 · 能源化学 · 催化科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Synthesis of polymetallic oxides hollow spheres with superior activity, resistance to SO2, H2O and metal poisons for low-temperature NH3‑selective catalytic reduction of NOx

Yu Zhang,Rui Wang

NH 3 ‑selective catalytic reduction as the fascinating technology for complete NO x removal, the key in practical applications is to explore advanced catalysts with high catalytic reactivity and stability at low temperature. Herein, a series of hollow spherical AMnO x (A = Ce, Cu, Ni) catalysts was fabricated by using carbon nanospheres as sacrificial template. Characterization analysis including XRD, ICP, BET, SEM, TEM, H 2 -TPR, NH 3 -TPD, XPS, in situ DRIFTS together with kinetic studies were applied to acquire knowledge of the morphological structure and surface features of the catalysts as-prepared. We also performed a comparative study on three samples with regard to their SCR activity at low temperatures. Notable, the catalytic activity of the NiMnO x catalyst (95.9 %) was vastly superior to that of the CeMnO x (85.4 %) and CuMnO x (30.5 %) at 100 °C. This enhanced low-temperature activity of NiMnO x are correlated against hollow structure with more active sites, wider pore distribution, higher surface Mn content and the enhancement in surface acidity and reducibility. Even with 5 vol% H 2 O in the reaction gas fraction, the catalytic performance of NiMnO x hollow spheres was superior to the other two catalysts. Besides, it can be used for six consecutive runs without suffering a substantial activity loss. Additionally, the impact of various crucial process variables, including space velocity, H 2 O, SO 2 , and metal poisons, on the denitrification efficiency of NH 3 -SCR was examined. The current researches have a positive guiding role in the development of high-efficiency low-temperature NH 3 -SCR denitrification catalysts to boost NO x degradation.

研究领域: 环境科学 · 催化化学
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2025 · IF 8.3

Embedded nanodiamonds into nitrogen-doped graphene aerogel anchoring palladium nanocrystallines enables efficient ethanol oxidation

Jing Li,Sizhuo Ma,Dingyuan Yi,Wenyu Chu,Yejie Wei,Jia Wei,Yanjun Cui,Shuwen Li

The increasing availability of active sites and optimizing electronic state of active metals are powerful strategies to rationally fabricate electrocatalysts with both high activity and long-term durability towards ethanol oxidation reaction (EOR). In this study, we fabricate a new catalyst, Pd nanocrystals (NCs) anchored on the embedded nanodiamonds (ND) into nitrogen-doped graphene (NG) aerogel (Pd/ND@NG). As an electrocatalyst for EOR in alkaline conditions, the optimized-Pd/ND@NG-2 achieves improved electrocatalytic activity (with a mass activity of 1338.0 mA mg −1 ) and reinforced poison resistance along with exceptional durability of minimal current decay after stability test, which are markedly surpassing those of commercial Pd/C (685.2 mA mg −1 ). Integrating the electrocatalytic measurements and systematic characterizations underscore the crucial roles of embedded ND into NG in enhancing electrocatalytic behavior of EOR. In brief, the embedded ND into NG observably increases the specific surface area and porosity of the prepared-electrocatalysts, which not only provides abundant channels for the mass/charge transfer but also increases the active sites availability through the high dispersion of small-sized Pd NCs on ND@NG supports. More importantly, the embedded ND into NG creates electron-deficient active Pd, which facilitates the adsorption of electron-rich intermediates (OH ads ) and the desorption of electron-deficient toxic intermediates (CO ads ), thereby boosting its electrocatalytic activity and durability. Additionally, this work provides an effective and practical strategy for assembling graphene aerogel, and offering insights for the development of research and application in electrocatalysis and beyond.

CAS / MDL: 31175-20-9
研究领域: 电催化 · 纳米材料 · 能源化学 · 表面科学 · 材料化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2025 · IF 21.1

Small-Size Atom-Driven Distortion Realizes High-Entropy Oxides with Simultaneous Chemical Stability and Activity Enhancement Enabling a Practical Cathode for Solid Oxide Fuel Cells

Wenjing Zhang,Wenjia Ma,Yuan Gao,Xu Han,Fangjun Jin,Ling Zhao,Kun Zheng,Yihan Ling,Peizhong Feng,Shaorong Wang,Zongping Shao

Both high activity for oxygen reduction reaction and excellent chemical stability against contaminants in the surrounding atmosphere under operating conditions are required for a viable cathode of solid oxide fuel cells. However, traditional Ba 0.8 Sr 0.2 Co 0.2 Fe 0.8 O 3-δ (BSCF) crystal structures suffer from instability under both high-temperature, high-reduction conditions and low-temperature, high-oxidation environments, making them prone to poisoning and significantly compromising their long-term operational stability. In this study, we engineered lattice distortion in BSCF by incorporating small-sized atoms at the A-site, resulting in a novel Ba 0.2 Sr 0.2 La 0.2 Pr 0.2 Sm 0.2 Co 0.2 Fe 0.8 O 3-δ (H-BSCF) high-entropy perovskite oxide, which shows significantly improved resistance to CO 2 and Cr vapor poisoning without impairing catalytic activity. Both experimental and results show the high-entropy strategy introduces lattice distortion, enhancing structural stability to prevent phase transitions and segregation. This distortion induces a spin state transition in Co 3+ ions that increases the density of unpaired electrons and significantly enhances Co 3d-O 2p orbital hybridization, which also prevent structural collapse, thereby markedly improving chemical stability without sacrificing catalytic activity. Density functional theory calculations demonstrate that H-BSCF possesses favorable oxygen migration energy and high segregation energy. The combined superior catalytic activity and stability make H-BSCF promising for industrial application.

研究领域: 材料科学 · 电化学 · 能源材料 · 固态离子学 · 催化化学
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