LANGMUIR
·
2021
·
IF 3.882
Jun Li,Xiaosi Liang,Liying Cai,Chenyang Zhao
Three-dimensional metallic nanonetworks (3D-MNWs) demonstrate unique performances across a wide range of fields, and their facile and green synthetic method is of high significance. Herein, we report a self-generated-nanobubble scaffolding strategy for the fabrication of 3D-MNWs, which employs aqua ammonia (AA) as a nanobubble reservoir and avoids the use of any surfactants or polymeric capping agents. Benefiting from the interaction between ammonia and metallic nanoparticles, finely interlocked nanonetworks (Au, Pt, Ag, and Cu) with curved geometry and abundant pores are obtained by precisely controlling the anisotropic kinetic growth using a strong reducing agent and a high concentration of AA. As a demonstration, the methanol oxidation reaction (MOR) is tested to assess the electrocatalytic performance of the Pt 3D-MNWs. The peak current of Pt 3D-MNWs reaches 152 mA/mgPt, which is 2.5 times higher than that of commercial Pt black. This unique nanobubble-assisted strategy has great potential in the basic synthetic prototype for polyporous nanomaterials.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Yihui Wu,Yuan Zhang,Yuxin Wang,Zhen He,Zhengjian Gu,Shuochao You
Ni–Fe–Sn electrocatalyst supported on nickel foam (Ni–Fe–Sn/NF) with high efficiency of hydrogen evolution reaction (HER) has been successfully fabricated through one-step potentiostatic electrodeposition route. The optimized Ni–Fe–Sn/NF displayed an extremely low overpotential of, respectively, 144 and 180 mV at 50 and 100 mA cm −2 for HER in alkaline condition. Moreover, it could retain its superior stability for at least 12 h. The remarkable electrocatalytic activity of our electrocatalyst is ascribed to the high conductivity originated from synergistic effects between Ni, Fe, and Sn during HER process.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yuhan Sun,Minghui Li,Xiaolei Qu,Shourong Zheng,Pedro J. J. Alvarez,Heyun Fu
A stable catalyst, Pt/carbon nanotube (CNT) coated with N-doped carbon (Pt/CNT@CN), was designed to reduce selenite (Se(IV)) in water to elemental selenium by liquid-phase catalytic hydrogenation. Commercial Pt/C, pristine Pt/CNT, and carbon-coated Pt/CNT (Pt/CNT@C) were used for benchmarking. The Pt particles in Pt/CNT@CN were completely embedded beneath the coatings to minimize leaching and were not easily accessible to Se(IV). However, Schottky–Mott-type metal–carbon junctions that activate H2 were formed on the coated catalyst, facilitating effective reduction of Se(IV). The initial activity of Pt/CNT@CN (900.5 mg L–1 gcat–1 h–1) was two times higher than that of commercial Pt/C (448.6 mg L–1 gcat–1 h–1). The commercial Pt/C and uncoated Pt/CNT lost their initial activities during reuse and were almost inactive after 10 cycles due to significant Pt leaching (>90%) during the reaction and acid-washing regeneration processes. Pt/CNT@CN maintained 33% of the initial activity after the first cycle and stabilized over the following 9 cycles due to effective protection of Pt particles by carbon coatings. After 10 cycles, the activity of Pt/CNT@CN was over 20 times higher than that of Pt/C and uncoated Pt/CNT. Overall, catalytic hydrogenation using carbon-coated-supported Pt catalysts is an effective and promising approach to remove Se(IV) in water.
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ChemistryOpen
·
2021
·Vol. 10
·期 5
·560-566
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IF 2.911
Yingshuang Hui,Yulu Zhan,Wenrong Hou,Lou Gao,Yahong Zhang,Yi Tang
Graphical The product control of C6 aldose toward C6, C4 and C2 alditols have been achieved, which have depended on the well-matched between retro-aldol condensation and hydrogenation process driving by temperature, H 2 pressure and injection modes. Alcohols have a wide range of applicability, and their functions vary with the carbon numbers. C6 and C4 alditols are alternative of sweetener, as well as significant pharmaceutical and chemical intermediates, which are mainly obtained through the fermentation of microorganism currently. Similarly, as a bulk chemical, C2 alditol plays a decisive role in chemical synthesis. However, among them, few works have been focused on the chemical production of C4 alditol yet due to its difficult accumulation. In this paper, under a static and semi-flowing procedure, we have achieved the product control during the conversion of C6 aldose toward C6 alditol, C4 alditol and C2 alditol, respectively. About C4 alditol yield of 20 % and C4 plus C6 alditols yield of 60 % are acquired in the one-pot conversion via a cascade retro-aldol condensation and hydrogenation process. Furthermore, in the semi-flowing condition, the yield of ethylene glycol is up to 73 % thanks to its low instantaneous concentration.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Rongcheng Mo,Xiaoran Zhang,Zhenyu Chen,Shangli Huang,Yanjie Li,Lizhe Liang,Zhi Qun Tian,Pei Kang Shen
Developing platinum-based nanoparticles on carbon catalysts with high activity and stability for oxygen reduction reaction (ORR) is of great significance for the practical application of fuel cells. Herein, a synchronous strategy of preparing nano-sized PtCo supported on atomic Co and N co-doped carbon nanorods (PtCo/Co–N–C NR) was developed to replace the conventional method of impregnating Pt sources into ready-made carbon materials , in which metal-organic frameworks (MOFs) with Co and Zn ions of rhombic dodecahedron were first prepared using 2-methylimidazole as building block and then their morphology was transformed into porous nanorods via the reduction of Co ions to Co–B–O complex in the MOFs by NaBH 4 ; subsequently, Pt was deposited on the Co–Zn MOF nanorods through the displacement reaction of PtCl 6 2 - and metallic Co and coordination between MOF and PtCl 6 2 - ; after pyrolysis and acid-leaching process, highly dispersed PtCo/Co–N–C NR was obtained. Attributed to its unique characteristics of hierarchical pore structure , uniform PtCo alloy nanoparticles with the average size of 7.0 nm and strong supporting interaction effect, the catalyst exhibits high ORR activity and stability with the mass activity of 577.0 mA mg −1 Pt and specific activity of 1.4 mA cm −2 at 0.9 V vs RHE in 0.1 M HClO 4 , which is about 3.6 times and 3.5 times high than that of commercial Pt/C catalyst respectively. This strategy would provide a flexible route to develop highly active and stable ORR electrocatalysts with various morphologies for optimizing the exposure of active sites.
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MICROCHEMICAL JOURNAL
·
2021
·
IF 4.821
Liya Zhou,Xitong Zhou,Congli Zhao,Yihang Liu,Yaoxuan Li,Li Ma,Ying He,Yanjun Jiang,Jing Gao
Molybdenum carbide (Mo 2 C) doping nitrogen nanoparticles (Mo 2 C/NCS) were synthesized by a facile and friendly method. Owing to the high surface area and structural tunability, Mo 2 C/NCS possesses the excellent electron conduction channels and exposes numerous active sites. Based on these characteristics, Mo 2 C/NCS was adopted to fabricate glassy carbon electrodes to construct acetylcholinesterase (AChE) biosensors for detecting organophosphorus pesticides (OPs). The prepared biosensors exhibited wide linear ranges from 1.0 × 10 −14 to 1.0 × 10 −6 M with the detection limit of 4.47 × 10 −15 M for malathion and 1.0 × 10 −13 to 1.0 × 10 −5 M with a limit of detection of 2.57 × 10 −14 M for methyl paraoxon. The AChE biosensor also displayed the outstanding stability and selectivity. The prepared AChE biosensor was also employed to detect OPs in cabbage and apple samples with high accuracies and satisfactory recoveries. Therefore, this study manifested a prominent transition metal carbides nanomaterial for biosensors in detecting OPs and provided a way for other enzyme-based biosensors.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Shaoda Huang,Shuanglong Lu,Hongyin Hu,Fangping Xu,Huining Li,Fang Duan,Han Zhu,Hongwei Gu,Mingliang Du
Although attentions have been devoted to developing Pd-based bimetallic nanocrystals towards the electrocatalytic oxygen reduction reaction (ORR) and ethanol oxidation reaction (EOR), the engineering of efficient bifunctional electrocatalysts with high atomic utilization still faces big challenges. Herein, we reported a facile one-pot template-free route to fabricate three-dimension hyper-dendritic PdZn nanocrystals (HD-PdZn NCs) that regulated by gas mixtures of carbon monoxide and hydrogen. The developed catalysts acted as robust bifunctional electrocatalysts for cathodic ORR and anodic EOR. Specifically, the engineered HD-PdZn NCs not only displayed superior mass activity (MA, 0.461 A mg Pd -1 ) and specific activity (SA, 0.393 mA cm −2 ) at 0.9 V, which were 5.2 and 5.0 times of commercial Pt/C, respectively, but also showed enhanced stability with only 3% loss of MA after 10,000 cycles for ORR. Density functional theory (DFT) calculations revealed the Zn implantation could facilitate the reduction of OOH* to OH* on the surface of Pd during the ORR process. Moreover, HD-PdZn NCs exhibited the highest EOR mass activity with a value of 3.45 A mg Pd −1 among benchmarked catalysts in alkaline solution. The advantageous structural features and electron effects are proposed to be responsible for the remarkable bifunctional activities. This work illustrates a facile method to fabricate highly efficient bifunctional electrocatalyst for energy conversation application.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Lin Zhong,Hu Zhou,Ruifeng Li,Hao Cheng,Sheng Wang,Boyuan Chen,Yongyue Zhuang,Junfeng Chen,Aihua Yuan
Developing highly efficient oxygen electrocatalysts is of vital importance for rechargeable Zn-air batteries (ZABs). Herein, Co/CoO x nano-heterojunctions encapsulated into nitrogen-doped carbon sheets (NCS@Co/CoO x ) are fabricated via a dual-template-guided approach by using zeolitic imidazolate frameworks (ZIFs) as templates. The synergistic integration of structural and compositional advantages endows such catalyst with superior catalytic properties to benchmark noble-metal catalysts. To be specific, the hierarchical micro/mesopores affords massive mass transport channels and maximizes the exposure of accessible active sites, whereas the NCS matrix accelerates electron transfer and prevents the self-aggregation of active species during the electrocatalytic reaction. Moreover, abundant and synergistic Co-based active sites (CoO, Co 3 O 4 , Co-N x ) greatly promote the catalytic activity. As the cathode of both liquid and flexible solid-state ZABs, excellent device properties are achieved, outperforming those assembled with commercial Pt/C+RuO 2 catalyst. This work presents a feasible and cost-effective strategy for developing oxygen electrocatalysts derived from ZIFs templates.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiaoning Wang,Xuejin Li,Tonghui Cai,Yongpeng Cui,Dongqing Kong,Jing Xu,Haoyu Hu,Yesheng Wang,Han Hu,Xiuli Gao,Yanpeng Li,Qingzhong Xue,Zifeng Yan,Lianming Zhao,Wei Xing
Designing electrocatalysts for hydrogen oxidation reaction (HOR) in alkaline media is crucial but challenging. Among all available electrocatalysts, Ni-based materials are recognized as the most potential precious-metal-free electrocatalysts for HOR. However, they still suffer from serious problems including low activity and poor stability. In this work, a synergistic chemical anchoring and electronic structure regulation strategy is proposed to gain both high electrocatalytic activity and stability for Ni-based HOR catalyst. N-doped graphite nanoflakes (N-GFs) support with abundant N anchoring sites can stabilize the loading of Ni-based active species, giving rise to an excellent stability of the catalyst. Meanwhile, the rationally designed heterostructure in the active Ni 3 N/Ni can trigger the electron transfer across the heterointerface, which optimizes the binding energy of the reaction intermediates, resulting in an accelerated the Volmer reaction. Benefited from the rational design, Ni 3 N/Ni/N-GFs exhibits excellent mass activity (42.7 A g Ni -1 at the overpotential of 50 mV) and stability (more than 24 h continuous operation). Moreover, the Ni 3 N/Ni heterostructure performs better in HOR electrocatalysis than individual Ni or Ni 3 N. These experimental results are rationalized by the theoretical simulations, which demonstrate that the heterostructure effectively weakens the hydrogen adsorption, optimizes the hydroxyl adsorption, and decreases the water formation reaction barrier.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2021
·
IF 4.464
Zhiyuan Lin,Wei Su,Song Zhang,Mingtao Zhang,Kexun Li,Jia Liu
A kind of Co 2 P embedded in nitrogen-doped carbon nanoframework (Co 2 PNC-NF) synthesized from directly carbonized Co-based metal-organic framework (ZIF-67) combined with phosphorus was utilized in the microbial fuel cell (MFC) to modify the active carbon air-cathode for the first time. Various techniques involving XRD, FESEM, TEM/EDS, BET and XPS were used to characterize the microstructure, morphology and surface chemical composition belonging to as-synthesized Co 2 PNC-NF. The electrochemical measurements revealed that the active carbon cathode modified by Co 2 PNC-NF got reduced resistance and optimized catalytic behavior in oxygen reduction reaction (ORR) process. The optimized MFC had a high maximum power density reaching 2001 mW m −2 , increasing by 123% compared with the bare active carbon cathode MFC. This result showed that combination between transition-metals phosphide and heteroatom-doped carbon matrices was beneficial to the improvement of MFC performance. Moreover, density functional theory calculations indicated that the special structure of double Co site of 001 face of Co 2 P can accelerate the ORR by boosting the cracking of OOH* group. Therefore, the Co 2 PNC-NF could be applied as an economical and efficient electrocatalyst in MFC to replace noble metal catalyst.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xibang Chen,Lang Sheng,Shuangxiao Li,Yu Cui,Tingrui Lin,Xueyan Que,Zhonghe Du,Zeyu Zhang,Jing Peng,Huiling Ma,Jiuqiang Li,Jingyi Qiu,Maolin Zhai
Transition metal phosphides (TMPs) have drawn considerable attention as a result of their high catalytic activities for the hydrogen evolution reaction (HER). In this work, a three-dimensional (3D) porous Co x P ordered nanoarray structure was successfully deposited on nickel foam (denoted as NF@Co x P, 1 ≦ x ≦ 2) via a strategy involving facile gamma ray irradiation and annealing without the use of reducing agent. By modulating the annealing temperature in the synthetic process for NF@Co x P, 3D porous ordered nanoarray composites exhibiting inherently superhydrophilic and superaerophobic properties were produced, the physical properties were confirmed with the use of various in-situ test techniques. The superhydrophilic properties of NF@Co x P help to increase the rate of ion transfer between the Co x P and the electrolyte. Additionally, in-situ verification of the superaerophobic properties showed that they are beneficial for quick release of the generated H 2 bubbles from the surface of NF@Co x P electrode, which was analyzed by coupling a 3D confocal microscope with an electrochemical workstation for the first time. As expected, when the resulting NF@Co x P composites were employed as catalyst electrodes for the HER in a 1 M KOH electrolyte, the 3D porous ordered nanoarray structure exhibited an overpotential of 272 mV at the current density of 200 mA cm −2 , which was much higher than those of commercial 20%Pt/C catalysts. Therefore, the synthetic strategy for producing NF@Co x P composites with 3D porous ordered nanoarray structures showed high potential for application in the HER.
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Small
·
2021
·Vol. 17
·期 34
·2101499
·
IF 13.281
Wen-Chao Geng,Yu-Jie Zhang,Lan Yu,Jing-Jing Li,Ji-Long Sang,Yong-Jun Li
To develop durable and low-price catalysts of methanol oxidation to commercialize direct methanol fuel cell, many attempts have been made at fabricating Pt-based hybrids by designing component-, morphology-, facet-, integration-pattern-varied nanostructures, and have achieved considerable successes. However, most of present catalysts still lack robust catalytic durability especially owing to the corrosion of mixed carbon and the poor mechanical stability of catalyst layer. Herein, Te nanowire array is transformed at an air/water interface into a 3D Pt 16 Te hierarchical nanostructure via an interface-confined galvanic replacement reaction. As-formed Pt 16 Te nanostructure has an asymmetrical architecture composed of nanotroughs and nanopillars, and nanopillars are perpendicular to nanotroughs with a loose arrangement. Pt 16 Te hierarchical nanostructure has a “self-supported” feature and, when directly used as the catalyst of methanol electrooxidation, exhibits superior catalytic activity (>four times larger in mass activity than state-of-the-art Pt/C in either acidic or basic solution) and long-term durability (after 500 cycles of cyclic voltammetric measurement, more than 55% of the initial specific activity remains whereas Pt/C only remains 22.2% in acidic solution and almost loses all activity in basic solution). This study fully demonstrates that designing “self-supported” catalyst film may be the next promising step for improving the catalytic performance of Pt-based hybrids.
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