ENVIRONMENTAL TECHNOLOGY
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2022
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IF 3.475
Zhen-xing Yang,Wen-yu Xie,Fang-fang Ye,De-hao Li
Electro-catalytic technology is a promising approach for wastewater treatment, owing to its easy operation, minimal generation of secondary pollution, small foot-print and rapid start-up. In this work, the chlorine evolution potential of the Pd-Sn modified ruthenium(Ru)-iridium(Ir) electrode was investigated for the electro-catalytic treatment of high chlorine ammonia-nitrogen wastewater. The effect of reaction conditions on the removal of ammonia-nitrogen, kinetics and apparent activation energy of ammonia-nitrogen removal were studied. The possible denitrification process of high chlorine ammonia-nitrogen wastewater was discussed. The results indicated that the chlorine evolution potential of the Pd-Sn modified Ru-Ir electrode was 1.0956 V(vs. SCE). The electro-catalytic treatment of high chlorine ammonia-nitrogen conformed to zero-order kinetic law, and the apparent activation energy of removal process was 14.089 kJ/mol. With a current was 0.5 A, the removal efficiency of ammonia-nitrogen could achieve 100% at a reaction time of 40 min. Indirect oxidation played an essential role in the electro-catalytic ammonia-nitrogen removal using the Pd-Sn modified Ru-Ir electrode. This paper demonstrated that the electro-catalytic technology was a promising approach for efficiently treating the high chlorine ammonia-nitrogen wastewater.
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Chemistry-An Asian Journal
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2022
·Vol. 17
·期 24
·e202200993
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IF 4.839
Zhijie Zhu,Xu Hu,Xingda An,Mengqi Xiao,Liang Zhang,Chaoran Li,Le He
Graphical The influence of the composition of bimetallic nanocrystals on their performance of photothermal catalytic CO 2 hydrogenation was investigated. Pd and Ni play different roles in the photothermal catalytic processes in the bimetallic system, which leads to a functional tradeoff over the stoichiometric ratio. Bimetallic nanomaterials exhibit excellent catalytic performance in photothermal CO 2 hydrogenation due to the synergistic effect between the two metal components. However, the component-performance relationship remains unclear, which hinders the design of efficient bimetallic catalysts and the investigation of catalytic reaction mechanism. Here we illustrate the influence of the composition of binary alloy on their performance of photothermal catalytic CO 2 hydrogenation by using monodispersed Pd−Ni nanocrystal as an example. Our study reveals that Ni and Pd play a significantly different role in the catalytic processes. Higher Ni component in the catalysts could lead to stronger light absorption, higher activity, and lower CO selectivity. The optimized Pd 4 Ni 1 −SiO 2 catalyst exhibited a near-unity and stable CO production rate of 230 mmol ⋅ g −1 ⋅ h −1 under 25-sun illumination. This study paves the way for the usage of bimetal in photothermal CO 2 catalysis towards more efficient solar-to-chemical energy conversions, and sheds light on some general design principles of bimetallic catalysts to balance the intrinsic properties of individual components.
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Nano Energy
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2022
·
IF 19.069
Bin Fang,Zipeng Xing,Weifeng Kong,Zhenzi Li,Wei Zhou
Electron spin polarization plays a vital role on photocatalysis but rarely considered. Herein, a double-layer hollow yolk-shell Pd/CoP@CoNiP superstructure photocatalyst is prepared via two ion exchanges approach using Co-MOF as a template. It shows ferromagnetic characteristics and obvious photothermal effect due to the special structure. Interestingly, the photocatalytic hydrogen evolution is enhanced about twice under external magnetic field compared to field-free. The improvement can be ascribed to the enhanced electron spin polarization of the vacancy defects for Pd/CoP@CoNiP superstructure and the formation of Z-scheme heterojunctions promoting efficient photogenerated charge separation and prolonging the lifetimes obviously. The special double-layer hollow yolk-shell superstructure is another reason for the optimized photocatalytic performance, which could expose adequate surface active sites for photocatalytic reaction. Moreover, the high stability of this defective Pd/CoP@CoNiP superstructure indicates the potential applications in field of photocatalysis. This strategy may provide new insights for fabricating high-efficient superstructure photocatalysts with electron spin polarization.
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CATALYSIS LETTERS
·
2022
·Vol. 153
·期 6
·1786-1796
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IF 2.936
Zhao Wei,Zhang Hongyi,Zhang Lei,Gong Jianchao,Chen Tianen,Ren Liming,Ji Yaxiong,Meng Fanbin
The methanol oxidation reaction is a promising route to eliminating trace amount of methanol in exhaust gases which aroused serious environmental concern. In this work, a novel Pd/MgAl 2 O 4 catalyst was prepared to construct the metal-support interface and employed in the methanol oxidation reaction. The reaction results show that the Pd/MgAl 2 O 4 catalyst could achieve 100% methanol oxidation at 198 ℃ over the Pd/MgO and Pd/Al 2 O 3 catalysts. The high-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), CO-chemisorption, H 2 temperature programmed reduction (H 2 -TPR), and CO diffuse reflectance infrared Fourier transformed spectroscopy (CO-DRIFTS) show that the Pd was uniformly distributed over the MgAl 2 O 4 support due to strong interaction between Pd and MgAl 2 O 4 . The mechanism studies show that the abundant Pd-MgAl 2 O 4 interfaces significantly contributed to the reaction enhancement. The Pd-MgAl 2 O 4 interfaces could greatly enhance the oxidation reaction at a lower temperature with the assistance of oxygen vacancies compared with traditional oxide catalysts, which was confirmed by methanol temperature program surface reaction (MeOH-TPSR) experiments. In-situ DRIFTS is carried out to elucidate the reaction mechanism and establish the structure − activity relationship: the methanol could be effectively absorbed on the MgAl 2 O 4 support with oxygen vacancies to form bidentate formate, then the Pd species assisted the intermediates converting to CO 2 product. The Pd/MgAl 2 O 4 catalyst and its enhancement mechanism investigation provided a potential strategy in the VOCs removal catalysis development. Graphical Abstract
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Mengjie Ma,Yi Zhang,Yujin Ji,Qi Shao,Kui Yin,Wenxiang Zhu,Junjun Yang,Fan Liao,Zhenglong Fan,Yang Liu,Youyong Li,Mingwang Shao,Zhenhui Kang
Poisoning species, such as methanol and air pollutants, degrade the electrocatalytic activity for oxygen reduction reaction (ORR). Here, via taking advantage of the varied electronic property of nano-silicon, a versatile strategy is reported for enhancing the catalytic activity and anti-poisoning ability toward ORR by decorating noble metal catalysts with the size-controlled silicon nanoclusters (DS). Consequently, DS-Pd exhibits the enhanced ORR performance with a large halfwave potential of 0.892 V and an onset potential of 1.010 V. More importantly, it also shows enhanced anti-poisoning performance in methanol, NaNO 2 and NaHSO 3 electrolytes, compared to those of commercial Pt/C and Pd/C catalysts. Mechanism studies reveal that the synergistic effect between Pd and more oxygen-philic and less poison-philic Si nanoclusters largely abbreviate the absorption of poisoning species on the active sites. This strategy also improves the methanol-tolerant performance of Pt based catalysts, providing a versatile strategy for the fabrication of methanol-tolerant ORR catalysts.
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Science China-Chemistry
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2022
·Vol. 65
·期 5
·877-884
·
IF 10.138
Li Zhenyu,Li Jiefei,Zheng Zexuan,Jiang Kunhong,Zheng Tianrun,Wang Dongmin,Wei Hang,Shi Zhiming,Li Xiaotian,Chu Haibin
In the field of noble metal-catalyzed alcohol electro-oxidation reaction (AOR), huge attention is paid on the composition, size, facet, and structure of the metals, while the support engineering should also be emphasized. CeO 2 has been widely used as an unique support in AOR, primarily due to its abundant oxygen vacancies (O v ). Herein, we report CeO 2 · x H 2 O nanoparticles with both massive hydroxyl groups (OH) and O v remarkably enhance the catalytic activity and stability of Pd toward ethanol oxidation reaction (EOR). The CO striping experiments and density functional theory (DFT) calculations suggest that OH and O v on CeO 2 · x H 2 O surface bring about a large downshift of Pd d-band center and a significant weakening of CO absorption on Pd. Moreover, OH and O v also play synergic roles in the removal of toxic intermediates. Consequently, the important roles of OH and O v of CeO 2 · x H 2 O are confirmed in Pd-catalyzed EOR. The facile CeO 2 · x H 2 O-enhanced strategy can contribute to the catalyst design for other energy conversion reactions.
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Materials Today Sustainability
·
2022
·
IF 7.244
X. Tai,B. Wu,J. Bao,W. Qu,L. Zhao,Z. Wang
Rational synthesis of bimetallic electrocatalysts with the special geometric structure for direct formic acid fuel cells remains yet challenging. Herein, a facile synthetic strategy is presented to prepare the bimetallic Pd–Cu alloy nanospheres (Pd–Cu ANSs) catalysts based on the galvanic replacement and high-temperature reconstruction. The formation mechanism of Pd–Cu ANSs is studied thoroughly from comprehensive characterizations and control experiments. The optimized Pd–Cu ANSs with unique nanosphere structure as well as regulated electronic structure provide excellent electrocatalytic performance for formic acid oxidation reaction (FAOR) with a specific activity of 6.11 mA cm - 2 Pd and mass activity of 1569.48 mA mg -1 Pd , which are 2.7 times and 3.5 times as high as these of the Pd/C catalyst. This synthetic method outlined here could provide a new pathway for noble metal-based alloy nanomaterials for diverse applications.
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CATALYSIS LETTERS
·
2022
·Vol. 152
·期 12
·3725-3732
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IF 2.936
Guo Pan,Zhan Yuzhong,Yang Yanliang,Lu Tianliang
The preparation of high-performance supported Pd catalysts for the hydrogenation of aromatic nitro is of great importance. In this paper, covalent-triazine framework (CTF), an organic porous crystalline material connected by covalent bonds, was employed as the support for the preparation of Pd heterogeneous catalyst. The framework of CTF was maintained due to the utilization of cyclohexene as a moderate reductant for PdCl 2 . The catalysts were characterized by transmission electron microscopy, energy-dispersive X-ray spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. The influence of reaction conditions (temperature, pressure, reaction time, concentration substrate and catalyst dosage) were investigated. At very mild reaction conditions (30 °C, 0.1 MPa H 2 , 2 mg Pd/CTF), the nitrobenzene was nearly stoichiometric hydrogenated to aniline. The Pd/CTF was effective for the conversion of a series of aromatic nitro compounds to the corresponding aromatic amines with good yield. The results showed that Pd/CTF has good catalytic activity and stability in the heterogeneous catalytic hydrogenation. Graphical Abstract
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JOURNAL OF RARE EARTHS
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2022
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IF 4.632
Rui Yang,Yunfeng Tian,Yun Liu,Jian Pu,Bo Chi
To promote the electrocatalytic activity and stability of traditional La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3– δ (LSCF) oxygen electrodes in reversible solid oxide cells (RSOCs), conventional physical mixed method was used to prepare the Pd-LSCF composite oxygen electrode. The cell with Pd-LSCF|GDC|YSZ|Ni-YSZ configuration shows perfect electrochemical performance in both solid oxide fuel cell (SOFC) mode and solid oxide electrolysis cell (SOEC) mode. In the SOFC mode, the cell achieves a power density of 1.73 W/cm 2 at 800 °C, higher than that of the LSCF oxygen electrode with 1.38 W/cm 2 . In the SOEC mode, the current density at 1.5 V is 1.67 A/cm 2 at 800 °C under 50 vol% steam concentration. Moreover, the reversibility and stability of the RSOCs were tested during 192 h long-term reversible operation. The degradation rate of the cell is only 2.2%/100 h and 2.5%/100 h in the SOEC and the SOFC modes, respectively. These results confirm that compositing Pd with the LSCF oxygen electrode can considerably boost the electrochemical performance of LSCF electrode in RSOCs field.
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Frontiers in Chemistry
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2022
·
IF 5.545
Liu Yangqing,Sun Jingwen,Fan Lan,Xu Qi
Subnanometer noble metal clusters have attracted much attention because of abundant low-coordinated metal atoms that perform excellent catalytic activity in various catalytic processes. However, the surface free energy of metals increases significantly with decreasing size of the metal clusters, which accelerates the aggregation of small clusters. In this work, new Schiff base–imidazole-functionalized MOFs were successfully synthesized via the postsynthetic modification method. Highly dispersed Pd clusters with an average size of 1.5 nm were constructed on this functional MOFs and behaved excellent catalytic activity in the Suzuki coupling of phenyboronic acid and bromobenzene (yield of biaryl >99%) under mild reaction conditions. Moreover, the catalyst can be reused six times without loss of activity. Such catalytic behavior is found to closely related to the surface functional groups that promote the formation of small Pd0 clusters in the metallic state.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
·
IF 7.2
Shijie Wang,Shenghan Zhang,Zhenye Zhang,Yu Tan,Kexin Liang,Xinliang Guo,Xuhui Kong
Nitrogen heterocyclic organics are promising hydrogen storage carriers with the advantage of being capable of large-scale transportation over long distances using existing oil and gas facilities. However, traditional methods for the hydrogenation and dehydrogenation of organic hydrogen carriers usually require high temperature and pressure conditions and external hydrogen supplies, which hinder their large-scale applications, as well as having certain safety risks. In this paper, a reversible electrochemical hydrogen storage system using quinoxaline as a hydrogen carrier was developed with potential for use at room temperature and atmospheric pressure. Experiments revealed that the hydrogenation conversion of quinoxaline reached 95% within 120 min at −0.20 V vs. RHE, and the dehydrogenation conversion of 1,2,3,4-tetrahydroquinoxaline reached 100% within 30 min at 1.30 V vs. RHE. This means that the system achieved quick and efficient reversible hydrogen storage. The Pd/NF dual-function electrode prepared by spontaneous redox reaction still showed high catalytic activity after 8 cycles, indicating its good long-term stability. The proton donor in the electrochemical hydrogenation process of quinoxaline was water, which completely eliminates the safety risk from the use of external hydrogen. This work provides a simple and reliable strategy for efficient hydrogen storage using nitrogen heterocyclic organics.
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Molecular Catalysis
·
2023
·
IF 4.6
Tianyun Cui,Yu Ling,Jipeng Meng,Ke Li,Changhai Liang,Chuang Li
Nowadays, the rational design of high-performance catalysts with desirable resistance to metal leaching has become the principal challenge in the hydrogenation of nitrile butadiene rubber. In the present work, the Pd-Pt bimetallic alloy nanocatalyst exhibits an outstanding hydrogenation degree of 99.0%, obviously higher than that of the conventional monometallic Pd/SiO 2 catalyst with the same Pd content (92.9%), accompanied by approximately 100% selectivity to C=C bonds. The results reveal that electron transfer from Pt to Pd confirms that the Pd species are in a rich-electron state, which boosts hydrogen activation and improves catalytic activity. Additionally, the incorporation of inactive Pt species promotes the formation of uniformly dispersed Pd-Pt alloy nanoparticles. The incorporation of inactive Pt species can enhance the metal-support interaction, reducing the residual metal content in hydrogenated nitrile butadiene rubber. The current research demonstrates a simple procedure for designing efficient bimetallic catalysts for the hydrogenation of unsaturated elastomer.
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