ACS Applied Materials & Interfaces
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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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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Jiawei Guo,Zhuojun Wei,Kun Wang,Hui Zhang
Novel CoFe-LDH (layered double hydroxide) nanosheet arrays in situ grown on rGO (reduced graphene oxide) uniformly modified Ni foam were synthesized by a citric acid-assisted aqueous phase coprecipitation strategy. Systematic characterizations indicates that the series of Co x Fe 1 -LDH/rGO/NF (x = 4, 3, 2) all show Co x Fe 1 -LDH nanosheets (150–180 × 15 nm) grown vertically on the surface of rGO/NF. Especially, the Co 3 Fe 1 -LDH/rGO/NF exhibits the best performance with overpotentials of 250 and 110 mV at 10 mA cm −2 in 1 M KOH for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), respectively. When it is used as cathode and anode simultaneously for overall water splitting, they require 1.65 and 1.84 V at 10 and 100 mA cm −2 , respectively. Excellent performance of Co 3 Fe 1 -LDH/rGO/NF is due to the nanosheet arrays structure with open channels, synergistic coupling between Co 3 Fe 1 -LDH and rGO enhancing electrical conductivity , and in-situ growth of Co 3 Fe 1 -LDH on rGO/NF enhancing stability.
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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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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Yikai Lu,Chenchen Liu,Shengjie Xu,Yu Liu,Deli Jiang,Jianjun Zhu
Designing and synthesizing stable, low-cost, and eco-friendly precious-metal-free electrocatalysts with high performance for hydrogen evolution is a critical and challenging task in the research and development of renewable hydrogen energy. Herein, we show an interfacial engineering strategy to synthesize the NiCoP nanosheets/NiCoP nanocubes homojunction electrocatalyst supported on Ni foam (2D/3D-NiCoP/NF). The as-synthesized 2D/3D-NiCoP/NF catalyst shows impressive HER activity, and a current density of 10 mA cm −2 can be achieved with only an overpotential of 37 mV in 1 M KOH solution. Such impressive HER performance of this 2D/3D-NiCoP/NF homojunction electrocatalyst is principally due to the exposure of abundance accessible active sites originated from the hierarchical structure of nanocubes on the nanosheets. Moreover, the intimate contact between 2D/3D-NiCoP and NF can simultaneously shorten the electron transport pathway and improve its stability. This novel 2D/3D-NiCoP/NF homojunction is expected to provide a powerful interface-engineering reference for the design and construction of high-efficiency synergistic HER electrocatalysts.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Xingru Yan,Sai Che,Fan Yang,Zhusong Xu,Hongchen Liu,Chenxuan Li,Lu Yan,Na Ta,Siyuan Sun,Qiang Wei,Lei Fang,Yongfeng Li
A non-noble-metal hybrid catalyst (Ni2P/NPC-P), composed of N,P-doped porous carbon decorated with surface P-enriched Ni2P nanoparticles, is developed to address the urgent challenges associated with mass production of clean hydrogen fuel. The synthesis features one-pot pyrolysis of inexpensive fluid catalytic cracking slurry, graphitic carbon nitride, and inorganic salts, followed by a feasible surface phosphidation process. As a non-noble metal catalyst, Ni2P/NPC-P demonstrates excellent performance in hydrogen evolution reaction in alkaline electrolytes with a low overpotential of 73 mV at a current density of 10 mA cm–2 (η10) and a small Tafel slope of 56 mV dec–1, meanwhile exhibits durability with no significant η10 change after 2000 catalytic cycles. Theoretical calculation reveals that the negatively charged P-enriched surface accelerated the rate-determining transformation and desorption of OH*. In overall water splitting, the electrocatalyst achieves a low η10 of 1.633 V, promising its potential in the cost-effective mass production of hydrogen fuel.
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IONICS
·
2021
·Vol. 27
·期 11
·4885-4895
·
IF 2.817
Qu Yuning,Yu Zehui,Wei Dan,Chen Ling,Zheng Zhe,Xiao Ningru,Wang Lili,Yu Jianguo
Pt-based materials have widely been explored as hydrogen evolution reaction (HER) catalysts, but the high cost of Pt catalyst limits its application in HER. Therefore, we report a platinum/polyvinyl-alcohol (Pt x -PVA) catalyst with high catalytic activity and low Pt loading. Pt x -PVA catalysts with a uniform distribution of the Pt nanoparticles (NPs) have successfully been synthesized by a simple one-step hydrothermal method. The size and morphology of Pt NPs can be easily adjusted by changing the amount of Pt precursor, easy to pick out the sample with the best performance. Among them, the Pt 1.88 -PVA catalyst exhibits the best electrocatalytic activity for HER in 0.5 M H 2 SO 4 solution. An overpotential of 34 mV on Pt 1.88 -PVA catalyst is obtained at a current density of −10 mA cm −2 , which is slightly better than the overpotential of the commercial Pt/C (42 mV). Similarly, the Tafel slope of 31 mV dec −1 on the Pt 1.88 -PVA catalyst indicates that the HER process is the Volmer-Tafel mechanism. However, the Pt loading of the Pt 1.88 -PVA catalyst is 18.8% times lower than that of the commercial Pt/C. Furthermore, the Pt x -PVA catalysts exhibit an excellent stability and durability. This is due to the coating effect of PVA for Pt NPs, which limits the migration and agglomeration of Pt NPs. This study provides a new approach for reducing the Pt load in Pt-based catalyst in the field of electrochemistry.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Yuning Qu,Zhe Zheng,Zehui Yu,Ming Song,Yanshuang Zhang,Yongnan Zhao,Jianguo Yu
In this study, chain-like PtPd/PVA catalysts were synthesized by a two-step hydrothermal method with the assistance of polyvinyl alcohol as a green reducing agent, structure guiding agent, dispersing agent , and binder. Among all the catalysts, Pt 1 Pd 5 /PVA catalyst shows the highest mass activity (3774.2 mA mg pt −1 ) for methanol oxidation reaction. Also, the residual activity of Pt 1 Pd 5 /PVA catalyst after chronoamperometry (CA) test of 28 h is close to that of commercial Pt/C after CA test of 5000 s. The excellent electrocatalytic activity of Pt 1 Pd 5 /PVA catalyst is mainly attributed to the synergistic effect between Pt and Pd. This can optimize the surface electronic structure and reduce the adsorption of CO-like species over the Pt surface. Besides, the unique chain network structure of PtPd forms a conductive network of self-conducting electrons. At the same time, a large amount of PVA causes an ultra-long stability through the coating of PtPd catalyst by PVA and the interaction with PVA and PtPd. This work contributes a facile and clean method for the synthesis of stable and efficient precious metal alloy catalysts for alcohols oxidation reaction .
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Xuefei Wu,Junxiang Chen,Zhenhai Wen
To explore highly active non-noble electrocatalysts toward full water splitting, the incorporation of other metal elements to the host electrocatalyst is required, especially for previously reported highly efficient MoO2–MoNi4 (MoNi in short). Herein, to lessen the energy cost in full water splitting, the vanadium-incorporated MoO2–MoNi4 (VMoNi in short) hybrid nanoarray self-supported on nickel foam is prepared through a simple way. Compared with the Mo–Ni binary electrocatalyst, vanadium incorporation can obviously boost oxygen evolution reaction (OER) activity while almost keeping the perfect hydrogen evolution reaction (HER) ability, for it merely requires 202 and 17 mV for 10 mA cm–2 working current density toward OER and HER, respectively. Furthermore, it displays outstanding performance toward full water splitting, merely requiring 1.45 V for 10 mA cm–2 and 1.61 V for 100 mA cm–2 in water electrolysis with keeping the voltage stable in tens of hours at 250 mA cm–2. This work highlights the significance in large-scale hydrogen production from water electrolysis with the help of exploring non-noble materials, an important milestone in converting the renewable energy to hydrogen energy.
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Arabian Journal of Chemistry
·
2021
·
IF 5.165
Yanping Chen,Qichao Zhao,Yanling Yao,Tianhao Li
Water electrolysis is a promising method for hydrogen production, so the preparation of low-cost and efficient electrocatalysts with a quick and simple procedure is crucial. Herein, iron phosphate (Fe 7 (PO 4 ) 6 ) was prepared via microwave radiation using ionic liquid (IL) as iron and phosphorus dual-source. This method is simple and rapid, and the product can be directly used as electrocatalysts without further treatment. The experimental results show that the IL can influence the morphology and electrocatalytic performance. Moreover, the addition of carbon nanotubes (CNTs) is favorable for formation of iron phosphate nanoparticles to improve the catalytic activities. As hydrogen evolution reaction (HER) catalyst, this iron phosphate/CNTs exhibits an onset overpotential of 120 mV, Tafel slope of 32.9 mV dec -1 , and current densities of 10 mA cm −2 at overpotential of 185 mV. Then, it obtains a good activity for oxygen evolution reaction (OER) with a low onset potential of 1.48 V, Tafel slope of 73.3 mV dec -1 , and it only needs an overpotential of 300 mV to drive the 10 mA cm −2 . This bifunctional catalyst also shows good durability for HER and OER. This microwave-assisted method provides an outstanding strategy to prepare iron phosphate in a simple and fast process with good catalytic performance for water splitting.
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Nanoscale
·
2019
·Vol. 12
·期 2
·973-982
·
IF 6.97
Jia-Jun Cai,Qing-Yan Zhou,Bing Liu,Xiao-Fei Gong,Yun-Long Zhang,Kokswee Goh,Da-Ming Gu,Lei Zhao,Xu-Lei Sui,Zhen-Bo Wang
Non-noble metal materials are regarded as the most promising catalysts for the oxygen reduction reaction (ORR) to overcome the inherent defects of Pt-based catalysts, like high cost, limited availability and insufficient stability. Here, we fabricate sandwich-like Co encapsulated nitrogen doped carbon polyhedron/graphene (s-Co@NCP/rGO) via a facile and scalable strategy by loading Co-based zeolitic imidazolate framework (ZIF-67) and graphene oxide (GO) layers individually on a polyurethane (PU) sponge template. The 3D sandwich structure is maintained with the assistance of the sponge template, which promotes the uniform dispersion of ZIF-67-derived Co embedded nitrogen doped carbon polyhedra (Co@NCP) and prevents the graphene plates from agglomerating during the annealing process. The final product demonstrates considerable catalytic performance for the ORR with a half-wave potential of 0.85 V, preferable stability and increased poisoning tolerance by comparison to 20 wt% Pt/C, which stems from the 3D sandwich-like structure, N/Co-doping effect, large accessible surface area and hierarchical porous structures. The excellent ORR performance of the catalysts means that they can be utilised in a Zn–air battery as cathode catalysts. During such a demonstration, s-Co@NCP/rGO shows a high open-circuit voltage of 1.466 V, remarkable long-term durability and an outstanding peak power density of 186 mV cm−2, which shows its high potential as a prospective alternative for widespread practical application in the field of non-noble metal ORR catalysts.
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Chemistry-An Asian Journal
·
2019
·Vol. 15
·期 1
·98-105
·
IF 3.698
Guohong Ren,Zhicheng Zhang,Yajun Liu,Ying Liang,Xichen Zhang,Shishan Wu,Jian Shen
Graphical Quaternary PtPdAuTe nanowires (NWs) with a rough surface were synthesized through a template method, and different atomic-ratio NWs were obtained by adjusting the amount of precursors. Electrochemical tests show that NWs have excellent activity for methanol oxidation. Multicomponent Pt-based nanowires (NWs) have attracted widespread attention as eletrocatalysts toward direct alcohol fuel cells because of their unique one-dimensional structure and high reaction dynamics. Quaternary PtPdAuTe NWs are designed via a facile template method, and NWs with a different composition are obtained by adjusting the feed ratio of metal precursors. The direct displacement reaction of metal precursors with Te NWs and the partial oxidation of Te lead to the formation of quaternary NWs. The rough surface and abundant reactive sites deriving from the rearrangement of metal atoms on the Te NWs surface endow the PtPdAuTe NWs with a superior electrocatalytic property and durability for methanol oxidation. The Pt 20 Pd 20 Au 10 Te 50 NWs display the largest mass activity and best stability among all catalysts. The preparation of PtPdAuTe NWs could provide a viable strategy for the preparation of other multicomponent NWs.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Ying Gao,Hanwei He,Wenyu Tan,Yizhi Peng,Xiaomei Dai,Yihui Wu
Exploring efficient, abundant, low-cost and stable materials for hydrogen evolution reaction (HER) is highly desired but still a challenging task. Herein, Ni–Se–Mo electrocatalysts supported on nickel foam (NF) substrate were synthesized by a facile one-step electrodeposition method. The Ni–Se–Mo film presents high electrocatalytic activity and stability toward HER, with a low overpotential of 101 mV to afford a current density of 10 mA cm −2 in 1.0 M KOH medium. Such excellent HER performance of Ni–Se–Mo film induced by the synergistic effects from Mo-doped Ni–Se film leads to the fast electron transfer . This work provides the validity of interface engineering strategy in preparing highly efficient transition metal chalcogenides based HER electrocatalysts.
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