INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
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
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传感器技术
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DOI
高影响因子
Nanoscale
·
2015
·Vol. 7
·期 17
·7615-7623
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IF 7.394
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
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催化化学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Minghu Zhao,Junyi Chen,Fei Wu,Yungang Wang,Kai Chen,Chao Xiong,Rongshu Zhu
Rationally designing catalysts suitable for flue gas purification at low temperatures and unraveling the anti-poisoning mechanism at the atomic level remain challenges. Here, a highly dispersed Ni-doped MnO x catalyst (Ni 0.1 Mn 0.9 O x ) was constructed and applied for selective catalytic reduction (SCR) of nitrogen oxides (NO x ). The long-term stability of Ni 0.1 Mn 0.9 O x is up to 80% (180 ℃) after 18 h under SO 2 and H 2 O conditions. This is due to the fact that the highly dispersed Ni atoms enhance the redox and surface acidity of MnO x , and modulate the electronic structure of the active Mn sites. The denitrification reaction on Ni 0.1 Mn 0.9 O x mainly follows the Eley-Rideal mechanism. The anti-poisoning mechanism is that the introduction of Ni weakens the electron transfer between the Mn site and SO 2 , thereby inhibiting the adsorption of SO 2 . In particular, the H 2 O adsorbed on the Ni sites is decomposed to replenish the depleted Brønsted acid sites, which facilitates the adsorption of NH 3 . However, an excess of H 2 O can have an inhibitory effect. In addition, the mesoporous structure may increase the mass transfer rate and reduce the accumulation of harmful substances. This study provides viable insights for the design of SCR catalysts with excellent anti-poisoning ability.
研究领域:
环境科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Shuke Huang,Jun Li,Yilan Chen,Liwei Yan,Peixin Zhang,Xueyan Zhang,Chenyang Zhao
In this work, we reported a novel polyphosphide strategy for the synthesis of phosphorus doped Pd (P-Pd) using red phosphorus as the starting material at quasi-ambient conditions. Polyphophide anions, as the key reaction intermediates, served as the reducing agent and phosphorus source to modulate the surface electronic structure of Pd. The P-Pd obtained exhibited topmost CO tolerance and electrocatalytic activity to formic acid oxidation among the state-of-arts reports. The mass activity and turnover frequency of P-Pd reached 4413 mA mg −1 Pd and 16.04 s −1 at 0.8 V, which were 23.7 and 6.4 times that of commercial Pd/C respectively. After 1000 repeated cycles, 82% initial activity was reserved. Combined with the electrochemical analysis and the density functional theory calculation, the boosted electrochemical performances can be attributed to the size and electronic effects induced by the P doping, which increase the surface actives sites, inhibit the adsorption of CO and change the reaction pathway to favorable CO 2 route. A full cell was also assembled to demonstrate the practical potential of the P-Pd, which showed a maximum power density of 21.56 mW cm −2 . This polyphophide-based reaction route provides a new strategy for the preparation of efficient and durable phosphorus doped alloys for electrocatalysis.
研究领域:
电催化
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材料科学
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能源化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Yongying Wang,Yangge Guo,Zhengwei Zhang,Zirui Wu,Chanez Maouche,Shuiyun Shen,Yi Li,Junliang Zhang,Juan Yang
Designing catalysts with high activity and stability to boost their ethanol oxidation reaction (EOR) performance is one of the central targets in the development of direct ethanol fuel cells (DEFCs). However, how to design the EOR catalysts in a rational way is still challenging, needing more efforts put in. Herein, we have synthesized a catalyst of PtCu-SnO 2 aerogel via ingeniously introducing Cu into Pt-SnO 2 system, resulting in the formation of a main phase of alloy (PtCu)-amorphous oxide (a-SnO 2 ) interface. Benefiting from the optimized structures, the PtCu-SnO 2 aerogel displays excellent acidic EOR performance with 4.5 times promotion in activity compared to pure Pt aerogel. In-depth investigations through electrochemical in-situ Fourier transform infrared spectroscopy and density functional theory calculations have shown that the absorbed OH on a-SnO 2 surface together with the greatly-modified electronic structure of the alloy surface atoms can facilitate the C1 pathway and the oxidation of *CO intermediates for ethanol oxidation reaction. The resulting affinity of surface OH and the modification of reaction energies both in turn contribute to the improvement of EOR performance with high activity, stability, and anti-poisoning ability, proving interfacial engineering an effective strategy for the rational design of EOR catalyst.
研究领域:
材料科学
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电化学
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催化科学
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产品关联
DOI
高影响因子
International Journal of Electrochemical Science
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2023
·
IF 1.5
Jun Li,Xiaosi Liang,Chenyang Zhao
Pd is a promising anodic catalyst for direct formic acid fuel cells, while its performance on formic acid electrooxidation is still suffered from for low catalytic efficiency and durability. In this work, an electrochemical self-catalyzed method was employed to deposit Au single-atoms onto Pd nanocrystals with tuneable compositions . Spherical-corrected Scanning transmission microscope and electrochemical characteristics demonstrated that the Au atoms were atomic-dispersive on Pd nanocrystals, forming Au-Pd single-atom alloy. Systematic studies showed that the activity of Pd x @Au y /C SAA is related to the density of the Au single-atoms on Pd surface. When an optimized balance between active-site exposure and intrinsic activity is achieved, the Pd 50 @Au 1 /C SAA showed superb formic acid electrooxidation activity of 4.98 A mg −1 M and unusual high anti-poisoning ability which is distinctly different from most of the Pd based catalysts. The boosted electrochemical performances of Pd x @Au y /C SAA can be attributed to the unique geometric effect that facilitates the direct reaction route and favourable electronic effect that weakens the CO adsorption to Pd sites.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
ELECTROCHIMICA ACTA
·
2025
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IF 5.6
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
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Dongping Fan,Ke Guo,Yan Zhang,Qiaoqiao Hao,Min Han,Dongdong Xu
High-entropy noble metals have attracted significant attention owning to their unique physicochemical characteristics. Here we report a simple method for the preparation of high-entropy PdPtCuAgAu nanowire networks using carboxyl-functionalized surfactants as soft templates. This PdPtCuAgAu alloy electrocatalysts possess synergetic compositional (e.g., high-entropy effect, sluggish diffusion effect, and lattice distortion effect) and structural (anisotropic and thin nanowires) advantages. The PdPtCuAgAu alloy electrocatalysts exhibit significantly enhanced electrocatalytic performance toward ethanol oxidation reaction, including high mass activity (7.7 A mg Pd+Pt −1 ), superior stability/durability, anti-poisoning ability, and fine electrocatalytic kinetics. Similar improvements in electrocatalytic performance are also seen in reactions involving other alcohols such as ethylene glycol and methanol. The high-entropy characteristics synergistically attributed to the enhanced electrocatalytic ability for different reaction process. This approach for the synthesis of high-entropy alloys will provide a new route to rationally design other high-entropy nanocatalysts with desired morphologies/structure and functions for a wide range of (electro)catalytic applications.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
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
✓ 已验证
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Jinxian Feng,Junyan Li,Lulu Qiao,Dong Liu,Pengfei Zhou,Jun Ni,Hui Pan
Zn-based materials are regarded as a family of promising electrocatalysts for electrochemical CO 2 reduction reaction (e-CO 2 RR), especially for the CO 2 -to-CO conversion. However, their electrocatalytic performances should be improved and the conversion mechanism needs to be further studied. In this work, we fabricate Cu-incorporated ZnO (Cu 25 Zn-A) on Zn plate for e-CO 2 RR catalyst by a facile annealing method. We find that Cu 25 Zn-A achieves a high CO Faraday efficiency > 90% with a CO yield rate of 0.49 mmol cm −2 h −1 . The improved catalytic activity on Cu 25 Zn-A is mainly attributed to the Cu steps on the reconstructed surface in the reaction: (1) that weakens the OH - /CO 3 2- adsorption, leading to the anti-poisoning surface by preventing the formation of Zn hydroxide/carbonates; and (2) that enhances the adsorption/activation of reactants and stabilizes the intermediates. Additionally, the density of defects in Zn oxide is increased by the Cu-incorporation, resulting in improved deoxygenation step. Our findings may provide insightful understanding on the mechanism and guide the design of novel electrocatalyst for effective CO 2 reduction.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2014
·
IF 2.235
Lu Lin,Tong Zhang,Xiongfu Zhang,Haiou Liu,King Lun Yeung,Jieshan Qiu
In this work, we fabricated a new type of Pd/SiO2@ZIF-8 core–shell catalyst composed of a Pd/SiO2 microsphere as the core and a ZIF-8 membrane as the shell. The preparation procedure involves first loading Pd nanoparticles onto nonporous SiO2 microspheres to obtain the Pd/SiO2 core and then coating a perfect layer of ZIF-8 shell on the core by electrostatic induction to form a Pd/SiO2@ZIF-8 core–shell structure. It is crucial that the modification of the Pd/SiO2 core with polyelectrolyte was employed to improve the charge distribution of the core surface and preferably adsorb Zn2+ cations in the synthesis solution so as to assist the formation of a continuous ZIF-8 shell. The compactness and thickness of the shell were optimized by increasing the number of cycles of ZIF-8 growth. The hydrogenations of alkenes with different molecular sizes showed that the Pd/SiO2@ZIF-8 catalysts can provide excellent product selectivity and antipoisoning and antileaching properties for the hydrogenations of alkenes.
研究领域:
催化
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Fei Wang,Kaili Wang,Chao An,Changhua An,Weiqing Zhang
Complete oxidation of ethanol is a pressing need for direct ethanol fuel cells (DEFCs) owning to high energy conversion. However, it holds great challenges on account of sluggish kinetics for C C bond cleavage and high susceptibility to CO poisoning. Herein, ternary PtPdCu nanocrsytals are synthesized and investigated for complete oxidation of ethanol. The obtained ternary PtPdCu nanodendrites (PtPdCu NDs) have a stepped surface, providing abundant active sites. Due to the structural and synergistic effects, ternary PtPdCu NDs exhibit a mass activity of 5.59 A mg PtPd −1 and specific activity of 15.82 mA cm −2 towards ethanol oxidation reaction, which are 6.4 and 3.6 times larger than that of commercial Pt/C. Further studies reveal that ternary PtPdCu NDs show strong abilities of CO anti-poisoning and C C bond cleavage, enhancing the C 1 pathway selectivity.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）