COLLOID AND POLYMER SCIENCE
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2017
·Vol. 295
·期 4
·703-707
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IF 1.723
Lu Wangting,Zhang Geng,Wei Feng,Li Wenhui,Cheng Kun,Ding Fei,Zhang Jiying,Zheng Wanquan
Palladium nanocrystals (NCs) are highly useful functional materials in many applications, and the performances of Pd NCs were strongly depended on the crystalline facet exposed on their surface. In this work, Pd NCs were synthesized in aqueous solutions by using Na 2 PdCl 4 as the precursor, citric acid as the capping agent, and Pluronic F127 as both stabilizer and reductant. By adjusting the reaction parameters, Pd cuboctahedrons, octahedrons, and triangular nanoplates with well-defined facets can be produced. This study provides a new pathway for the shape-controlled preparation of noble metal NCs.
研究领域:
材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2017
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IF 3.582
Nan Jia,Yaru Shi,Shuxia Zhang,Xinbing Chen,Pei Chen,Zhongwei An
The carbon supporting materials play a crucial role for improving the utilization and electrocatalytic activity of noble metal nanocrystals . In this work, the high-quality carbon nanobowls (CNBs) with high surface area are synthesized successfully by a simple sol–gel synthetic method. Then, the as-prepared CNBs are used as advanced supporting material to anchor Pd nanocrystals by a facile homogeneous precipitation–reduction method. The as-prepared CNBs supported Pd nanocrystals (Pd/CNBs) nanohybrids are examined thoroughly by various physical characterizations . Physical measurements display that the CNBs facilitate the dispersion and anchorage of Pd nanocrystals due to their high surface area and abundant O-containing surface groups. Cyclic voltammetry , electrochemical impedance spectroscopy , and chronoamperometry measurements reveal that the Pd/CNBs nanohybrids have higher electrocatalytic activity and durability for the formic acid electro oxidation than Vulcan XC-72 carbon supported Pd nanocrystals (Pd/C-72) nanohybrids and commercial Pd/C electrocatalyst .
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
Progress in Natural Science-Materials International
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2016
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IF 1.753
Yu Bai,Chunlei Wang,Xingyi Zhou,Junling Lu,Yujie Xiong
Pd typically exhibits relatively low catalytic activity in CO oxidation, as CO is apt to be adsorbed on Pd to poison the surface for O 2 activation. In this Letter, we report that this limitation can be overcome by integrating Pd with TiO 2 . The TiO 2 was coated on Pd nanocubes with a controllable thickness using atomic layer deposition (ALD) method. Given the different work functions of TiO 2 and Pd, the electrons in TiO 2 semiconductor will flow toward Pd. With the electron density increased on Pd, the adsorption of CO to Pd will be weakened while the oxygen activation can be facilitated. Meanwhile, the interface-confined sites at Pd-TiO 2 may further enhance the oxygen activation. As the species adsorption and activation are strongly correlated with electron density, the performance of Pd-TiO 2 in CO oxidation turns out to depend on the TiO 2 thickness, which determines the number of transferred electrons, within a certain range (<1.8 nm). This work provides a new strategy for enhancing catalytic performance through tailoring charge densities in hybrid catalysts.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
Nano Research
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2015
·Vol. 8
·期 6
·2115-2123
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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.
研究领域:
材料科学
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催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Yi Han,Xinyi Zhang,Wenwen Cai,Huan Zhao,Yanyun Zhang,Yuyao Sun,Zhiqiang Hu,Shaoxiang Li,Jianping Lai,Lei Wang
Electrochemical nitrate reduction reaction (NO 3 − RR) is considered an appealing way for producing ammonia (NH 3 ) under ambient conditions and solving environmental problems caused by nitrate, whereas the lack of adequate catalysts hampers the development of NO 3 − RR. Here, we firstly demonstrate that the Pd nanocrystalline with a well-desired facet can act as a highly efficient NO 3 − RR electrocatalyst for ambient ammonia synthesis. Pd (1 1 1) exhibits excellent activity and selectivity in reducing NO 3 − to NH 4 + with a Faradaic efficiency of 79.91% and an NH 4 + production of 0.5485 mmol h −1 cm −2 (2.74 mmol h −1 mg −1 ) in 0.1 M Na 2 SO 4 (containing 0.1 M NO 3 − ), which is 1.4 times higher than Pd (1 0 0) and 1.9 times higher than Pd (1 1 0), respectively. Density functional theory (DFT) calculation reveals that the superior NO 3 − RR activity of Pd (1 1 1) originates from its optimized activity of NO 3 − adsorption, smaller free energy change of the rate-limiting step (*NH 3 to NH 3 ), and poorer hydrogen evolution reaction activity (HER, competitive reaction). This work not only highlights the potentials of Pd-based nanocatalysts for NO 3 − RR but also provides new insight for the applications in NO 3 − RR of other facet-orientation nanomaterials.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
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2022
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IF 5.089
Yuwen Wang,Zenghui Bi,Xue Zhao,Abdukader Abdukayum,Shuxing Zhou,Haibo Zhang,Jianbing Chen,Fang Tan,Anran Chen,Thomas Wågberg,Guangzhi Hu
The reduction of nitroaromatics to aminoaromatics is essential for fine chemical production and effective sewage treatment. However, the activity of an external catalyst is essential for the reaction. In this study, Pd nanocrystals were anchored in situ on two-dimensional graphene oxide (GO), which acted as a catalyst support with high specific surface area. The oxygen-containing groups on the surface of GO bonded to the functionally rich boron clusters through hydrogen bonding interactions. A mildly reducible closed-dodecahydrododecaboric acid anion cluster ( closo‑ [B 12 H 12 ] 2– ) was employed as the target site. The mild reducibility of closo‑ [B 12 H 12 ] 2– resulted in a wide dispersion of ultrafine Pd nanocrystals on GO. Under ambient conditions, Pd/BGO rapidly hydrogenated nitroaromatics, such as 4-nitrophenol, to aminoaromatics with approximately 100% efficiency. Moreover, Pd/BGO retained its high catalytic activity for the hydrogenation/reduction of 4-nitrophenol after five catalytic cycles. Therefore, Pd/BGO could be a promising and economically viable candidate for various practical applications. The proposed innovative preparation strategy and highly efficient catalytic activity suggested the effective performance of closo‑ [B 12 H 12 ] 2– as nanometal nucleation target sites. In addition to providing an alternate route for preparing supported nanometals, this study presents a stable and efficient catalyst for the hydrogenation of nitroaromatics.
研究领域:
化学工程
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材料科学
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催化技术
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Mingna Chu,Kai Cui,Yan Zhou,Xiuzhi Yuan,Wei Qin,Yang Li,Xiaohong Wu
Enhancing the photoreduction of carbon dioxide (CO 2 ) to produce valuable chemicals, such as carbon monoxide (CO), is of significant importance. The bottleneck in developing advanced catalysts lies in the rational design of catalytic centers with efficient CO 2 activation and hydrogen proton production. In this work, palladium nanoparticles (Pd NPs) were successfully modified on UiO-66-NH 2 -Zn SAs (UN-Zn SAs) by a photo-deposition method. The optimized photocatalyst , 4 Pd NPs-UN-0.7Zn SAs, demonstrated exceptional performance in converting CO 2 to CO, exhibiting approximately 1.4-fold and 7.8-fold enhancements compared to UN-0.7Zn SAs and UN, respectively. A combination of time-resolved photoluminescence spectroscopy and electron paramagnetic resonance results unveiled that the introduction of Pd NPs effectively promoted the photogenerated charge separation and facilitated water activation to produce more hydrogen protons. The generated hydrogen protons were subsequently coupled with nearby CO 2 that was activated by Zn SAs, thus achieving the facile water-activation-induced CO 2 reduction process. Theoretical calculations further confirmed that the heterogeneous synergistic effects between Zn SAs and Pd NPs lowered the energy barrier for the rate-limiting step of CO 2 conversion to COOH* , thereby achieving efficient photocatalytic CO 2 reduction reactions. This work provides a new perspective on the development of efficient catalysts for the effective conversion of CO 2 .
研究领域:
化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2022
·
IF 7.392
Xue Li,Xue Zhao,Yingtang Zhou,Jiao Hu,Hucai Zhang,Xun Hu,Guangzhi Hu
Ammonia is used extensively as a raw material for fertilizers and industrial production. However, the ammonia yield of the traditional ammonia production process is far from reaching the requirements of industrial applications. Among various methods, electrochemical ammonia synthesis is the most anticipated. Density functional theory (DFT) calculations show that nanoscaled palladium (Pd) decorated on boron–carbon-nitrogen (BCN) support has great catalytic activity towards nitrate electrochemical reduction. We designed and synthesized the BC2N/Pd (both B and N atomic loading more than 20%) electrocatalysts and applied them to electrochemically convert harmful nitrate to high value-added ammonia, which performed an excellent ammonia yield rate of 1730 μg h −1 cm −2 and a high Faraday efficiency of 97.42% in water that containing 250 mM KNO 3 . Isotope labeling experiments proved that ammonia originates from nitrate reduction. At the same time, BC2N/Pd also exhibits splendid stability and durability. The outstanding electrocatalytic activity suggests good prospects in industrial applications, including the purification of ammonia and nitrate wastewater.
研究领域:
材料科学
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环境科学
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催化化学
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 31
·期 4
·2006853
·
IF 16.836
Jiajie Chen,Shiyang Lin,Doudou Zhao,Lei Guan,Yaping Hu,Yitong Wang,Kaili Lin,Yufang Zhu
Hydrogen therapy, as a star therapeutic modality, has recently acquired much attention in the field of anticancer medicine. Evidence suggests that hydrogen can selectively reduce intratumoral overexpressed hydroxyl radicals (•OH) to break the redox homoeostasis and thereby result in redox stress and cell damage. As a reactive oxygen species-related noninvasive modality, photodynamic therapy (PDT) has been approved for varied tumor treatments clinically. For implementing tumor therapy with enhanced anticancer efficacy and attenuated side effects, here a biocompatible palladium nanocrystals-integrated nanoscale porphyrinic metal–organic framework (NPMOF) is designed to develop a novel combined therapy modality, that is, synergistic hydrogen/photodynamic therapy. The NPMOF is employed simultaneously as the photosensitizer for PDT and as the nanocarrier to support palladium nanocrystals, which is further used as the hydrogen vehicle. The final hydrogen-containing nanosystems exhibit a persistent reductive hydrogen release behavior and considerable light-activated singlet oxygen ( 1 O 2 ) generation without mutual interference, contributing to the adequate disturbance of tumor microenvironment redox steady-state for synergistically inducing tumor cell death. Ultimately, by coupling of tumor-selective hydrogen therapy and PDT, the designed nanosystems realize the augmented therapeutic outcome with minimal side effects, providing a safe and efficient tumor treatment for future clinical translation.
研究领域:
生物医学工程
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肿瘤学
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纳米医学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Ding Wang,Jialin Yang,Liping Bao,Yu Cheng,Liang Tian,Qingxiang Ma,Jingcheng Xu,Hui-Jun Li,Xianying Wang
Hydrogen (H 2 ) molecules are easy to leak during production, storage, transportation and usage. Because of their flammability and explosive nature, quick and reliable dectection of H 2 molecule is of great significance. Herein, an excellent H 2 gas sensor has been realized based on Pd nanocrystal sensitized two-dimensional (2D) porous TiO 2 (Pd/TiO 2 ). The formation of 2D porous TiO 2 with the removal of graphene oxide template has been monitored by an in-situ transmission electron microscope. It is found that the size of the GO template can be almost completely replicated by 2D TiO 2 . The Pd/TiO 2 sensor exhibited an instantaneous response and a satisfactory low detection limit for H 2 detection. These excellent gas-sensing performances (good selectivity, unique linearity response and high stability) can be attributed to the unique 2D porous structure and the synergistic effect between oxidized Pd and TiO 2 , including the unique adsorption properties of O 2 or/and H 2 on Pd/TiO 2 , the reaction between PdO and H 2 gas, and the regulated depletion layer arising from p-type PdO to n -type TiO 2 . This work demonstrates a rational design and synthesis of highly efficient H 2 sensitive materials for energy and manufacturing security.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2025
·
IF 7.9
Jinjuan Zhao,Sizhuo Ma,Aoxue Zhang,Yuner Xu,Zheng Liu,Mengjie Li,Honglei Yang,Ruifa Jin,Shuwen Li
The hydrogen-bonding interaction among catalytic center, support material and ethanol molecule can establish an effective microenvironment for ethanol oxidation reaction (EOR). However, the surrounding of palladium nanocrystals (Pd NCs) lacks highly electronegative atoms to form hydrogen bonds with ethanol molecule. To effectively address the limitation, suitable molecules can be incorporated into Pd-based catalysts alongside the selection of an appropriate support. The pyrene tetracarboxylate ionic liquid (PTCIL), composed of pyrene tetracarboxylate anions and quaternary ammonium cations, provides abundant oxygen atoms capable of forming hydrogen bonds with ethanol molecules and the oxygen-containing functional groups in reduced graphene oxide (RGO) support, thereby creating a conducive microenvironment towards green EOR. Additionally, PTCIL can be anchored onto the RGO support via π-π stacking, yielding abundant dispersed carboxyl and pyrenyl groups that act as active sites to stabilize Pd NCs. Furthermore, synergistic interactions within the catalyst enable electron transfer from PTCIL to Pd, weakening the adsorption strength of toxic intermediates. Herein, the prepared Pd/PTCIL-RGO-2 exhibits improved electrocatalytic activity (1523.2 mA mg −1 , 5.29 mA cm −2 ) compared to commercial Pd/C (807.2 mA mg −1 , 4.14 mA cm −2 ). This study proposes a design for constructing Pd-based catalysts with tailored local microenvironments, exhibiting enhanced activity and robust durability for versatile applications, including EOR and other small molecule oxidation reactions.
研究领域:
电催化
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材料化学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2020
·
IF 8.758
Yang Yang,Jiachang Zeng,Yijin Shu,Qingsheng Gao
Noble-metal nanocrystals (NCs) are functional segments of biosensing platforms, but their sensitivity and facet effects are still challenging. Conventional synthesis using surfactants to direct crystal growth unfortunately causes adsorbate–surface hindrance, which not only reduces sensing responses but also leads to misunderstanding on facet-dependence. Herein, we utilize electrochemical CO displacement to remove residual surfactants from facet-engineered Pd NCs, and further investigate the structure–activity relationship on specific facets, for example, {100} in cubes, {111} in octahedrons, and {110} in rhombic dodecahedrons. Along with the remarkably boosted response, facet dependence is obvious for H2O2 sensing after surface cleaning. The Pd{100} shows high sensitivity, low detection limit, and wide applicable concentration range, superior to the {110} and {111}. This can be theoretically interpreted by the befitting *OH binding on {100} and thereby the facilitated H2O2 reduction kinetics. The outstanding selectivity to H2O2 ensures the high efficiency of Pd NCs to measure intracellular H2O2 and recognize different types of cancer cells. Moreover, facet effects are also evidenced in glucose detection, highlighting that this work can provide guidelines to design efficient sensing platforms.
研究领域:
材料科学
·
分析化学
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生物医学工程
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）