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1.
Dr. Chakadola Panda Dr. Prashanth W. Menezes Prof. Dr. Matthias Driess 《Angewandte Chemie (International ed. in English)》2018,57(35):11130-11139
The low‐temperature synthesis of inorganic materials and their interfaces at the atomic and molecular level provides numerous opportunities for the design and improvement of inorganic materials in heterogeneous catalysis for sustainable chemical energy conversion or other energy‐saving areas. Using suitable molecular precursors for functional inorganic nanomaterial synthesis allows for facile control over uniform particle size distribution, stoichiometry, and leads to desired chemical and physical properties. This Minireview outlines some advantages of the molecular precursor approach in light of selected recent developments of molecule‐to‐nanomaterials synthesis for renewable energy applications, relevant for the oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and overall water‐splitting. 相似文献
2.
Yong‐Sheng Wei Liming Sun Miao Wang Jinhua Hong Lianli Zou Hongwen Liu Yu Wang Mei Zhang Zheng Liu Yinwei Li Satoshi Horike Kazu Suenaga Qiang Xu 《Angewandte Chemie (International ed. in English)》2020,59(37):16013-16022
Understanding the thermal aggregation behavior of metal atoms is important for the synthesis of supported metal clusters. Here, derived from a metal–organic framework encapsulating a trinuclear FeIII2FeII complex (denoted as Fe3) within the channels, a well‐defined nitrogen‐doped carbon layer is fabricated as an ideal support for stabilizing the generated iron nanoclusters. Atomic replacement of FeII by other metal(II) ions (e.g., ZnII/CoII) via synthesizing isostructural trinuclear‐complex precursors (Fe2Zn/Fe2Co), namely the “heteroatom modulator approach”, is inhibiting the aggregation of Fe atoms toward nanoclusters with formation of a stable iron dimer in an optimal metal–nitrogen moiety, clearly identified by direct transmission electron microscopy and X‐ray absorption fine structure analysis. The supported iron dimer, serving as cooperative metal–metal site, acts as efficient oxygen evolution catalyst. Our findings offer an atomic insight to guide the future design of ultrasmall metal clusters bearing outstanding catalytic capabilities. 相似文献
3.
Dr. Yong-Sheng Wei Dr. Liming Sun Miao Wang Dr. Jinhua Hong Dr. Lianli Zou Hongwen Liu Dr. Yu Wang Dr. Mei Zhang Dr. Zheng Liu Prof. Yinwei Li Prof. Satoshi Horike Prof. Kazu Suenaga Prof. Qiang Xu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(37):16147-16156
Understanding the thermal aggregation behavior of metal atoms is important for the synthesis of supported metal clusters. Here, derived from a metal–organic framework encapsulating a trinuclear FeIII2FeII complex (denoted as Fe3) within the channels, a well-defined nitrogen-doped carbon layer is fabricated as an ideal support for stabilizing the generated iron nanoclusters. Atomic replacement of FeII by other metal(II) ions (e.g., ZnII/CoII) via synthesizing isostructural trinuclear-complex precursors (Fe2Zn/Fe2Co), namely the “heteroatom modulator approach”, is inhibiting the aggregation of Fe atoms toward nanoclusters with formation of a stable iron dimer in an optimal metal–nitrogen moiety, clearly identified by direct transmission electron microscopy and X-ray absorption fine structure analysis. The supported iron dimer, serving as cooperative metal–metal site, acts as efficient oxygen evolution catalyst. Our findings offer an atomic insight to guide the future design of ultrasmall metal clusters bearing outstanding catalytic capabilities. 相似文献
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MOF‐Derived Hollow CoS Decorated with CeOx Nanoparticles for Boosting Oxygen Evolution Reaction Electrocatalysis 下载免费PDF全文
Huajie Xu Prof. Jing Cao Changfu Shan Bingkai Wang Prof. Pinxian Xi Prof. Weisheng Liu Prof. Yu Tang 《Angewandte Chemie (International ed. in English)》2018,57(28):8654-8658
Transition‐metal sulfides (TMSs) have emerged as important candidates for oxygen evolution reaction (OER) electrocatalysts. Now a hybrid nanostructure has been decorated with CeOx nanoparticles on the surface of ZIF‐67‐derived hollow CoS through in situ generation. Proper control of the amount of CeOx on the surface of CoS can achieve precise tuning of Co2+/Co3+ ratio, especially for the induced defects, further boosting the OER activity. Meanwhile, the formation of protective CeOx thin layer effectively inhibits the corrosion by losing cobalt ion species from the active surface into the solution. It is thus a rare example of a hybrid hetero‐structural electrocatalyst with CeOx NPs to improve the performance of the hollow TMS nanocage. 相似文献
6.
A Molecular Approach to Manganese Nitride Acting as a High Performance Electrocatalyst in the Oxygen Evolution Reaction 下载免费PDF全文
Carsten Walter Dr. Prashanth W. Menezes Steven Orthmann Jona Schuch Paula Connor Dr. Bernhard Kaiser Prof. Dr. Martin Lerch Prof. Dr. Matthias Driess 《Angewandte Chemie (International ed. in English)》2018,57(3):698-702
The scalable synthesis of phase‐pure crystalline manganese nitride (Mn3N2) from a molecular precursor is reported. It acts as a superiorly active and durable electrocatalyst in the oxygen evolution reaction (OER) from water under alkaline conditions. While electrophoretically deposited Mn3N2 on fluorine tin oxide (FTO) requires an overpotential of 390 mV, the latter is substantially decreased to merely 270 mV on nickel foam (NF) at a current density of 10 mA cm?2 with a durability of weeks. The high performance of this material is due to the rapid transformation of manganese sites at the surface of Mn3N2 into an amorphous active MnOx overlayer under operation conditions intimately connected with metallic Mn3N2, which increases the charge transfer from the active catalyst surface to the electrode substrates and thus outperforms the electrocatalytic activity in comparison to solely MnOx‐based OER catalysts. 相似文献
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The incident photon to current efficiency (IPCE) of a photoactive surface strongly depends on the loading and thickness of the active materials. We present a combinatorial approach based on an optical scanning droplet cell for simultaneous deposition and systematic characterization of co‐catalysts for the oxygen evolution reaction (OER) on Mo‐doped BiVO4 (Mo?BiVO4) photoanodes electrochemically pre‐deposited on transparent conductive FTO substrates. The loading and photoelectrochemical characterization of 10 different OER co‐catalysts deposited by three different deposition techniques on FTO‐supported Mo?BiVO4 were investigated aiming at determination of the suitable deposition parameters affording the highest enhancement of photoelectrochemical oxygen evolution for the different OER/Mo?BiVO4 films. A comparison of the photoelectrochemical performance of films of various OER co‐catalyst deposited on FTO‐supported Mo?BiVO4 by electrodeposition, photo‐assisted electrodeposition and photodeposition revealed the necessity of a material specific optimization with respect to co‐catalyst loading and deposition technique to achieve optimal IPCE for each co‐catalysts. 相似文献
8.
Rui‐Juan Xiang Prof. Dr. Hong‐Yan Wang Zhi‐Juan Xin Dr. Cheng‐Bo Li Ya‐Xing Lu Dr. Xue‐Wang Gao Dr. Hua‐Ming Sun Prof. Dr. Rui Cao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(5):1602-1607
The water‐soluble polypyridine copper complex [Cu(F3TPA)(ClO4)2] [ 1 ; F3TPA=tris(2‐fluoro‐6‐pyridylmethyl)amine] catalyzes water oxidation in a pH 8.5 borate buffer at a relatively low overpotential of 610 mV. Assisted by photosensitizer and an electron acceptor, 1 also exhibits activity as a homogeneous catalyst for photo‐induced O2 evolution with a maximum turnover frequency (TOF) of (1.58±0.03)×10?1 s?1 and a maximum turnover number (TON) of 11.61±0.23. In comparison, the reference [Cu(TPA)(ClO4)2] [TPA=tris(2‐pyridylmethyl)amine] displayed almost no activity under either set of conditions, implying the crucial role of the ligand in determining the behavior of the catalyst. Experimental evidence indicate the molecular catalytic nature of 1 , leading to a potentially practical strategy to apply the copper complex in a photoelectrochemical device for water oxidation. 相似文献
9.
《化学:亚洲杂志》2017,12(4):446-452
Here we report a redox‐anchoring strategy for synthesizing a non‐noble metal carbide (MoCx) nanocomposite electrocatalyst for water electrolysis in acidic media, using glucose and ammonium heptamolybdate as carbon and Mo precursors, respectively, without the need of gaseous carbon sources such as CH4. Specifically, the aldehyde groups of glucose are capable of reducing Mo6+ to Mo4+ (MoO2), and thus molybdenum species can be well anchored by a redox reaction onto a carbon matrix to prevent the aggregation of MoCx nanoparticles during the following carbonization process. The morphology and chemical composition of the electrocatalysts were well characterized by BSE‐SEM, TEM, XRD and XPS. The obtained MoCx−2 sample showed a reasonably high hydrogen evolution reaction (HER) activity and excellent stability in an acidic electrolyte, and its overpotential required for a current density output of 20 mA cm−2 is as low as 193 mV. Such a prominent performance is ascribed to the excellent dispersity and nano‐size, and the large reactive surface area of MoCx particles. This work may open a new way to the design and fabrication of other non‐noble metal carbide nanocatalysts for various electrochemical applications. 相似文献
10.
Prussian Blue‐Derived Iron Phosphide Nanoparticles in a Porous Graphene Aerogel as Efficient Electrocatalyst for Hydrogen Evolution Reaction 下载免费PDF全文
Dr. Narendra Kumar Alam Venugopal Shuli Yin Yinghao Li Dr. Hairong Xue Dr. You Xu Prof. Xiaonian Li Dr. Hongjing Wang Prof. Liang Wang 《化学:亚洲杂志》2018,13(6):679-685
Tailoring of new hydrogen evolution reaction (HER) electrocatalyst with earth abundant elements is important for large scale water splitting and hydrogen production. In this work, we present a simple synthetic method for incorporating iron phosphide (FeP) particles into three‐dimensional (3D) porous graphene aerogel (GA) structure. The FeP formed in porous 3D GA (FeP/GA) is derived from electroactive Fe hexacyanoferrate (FeHCF). The advantage of incorporating FeP, in the porous 3D graphene network enables high accessibility for HER. As synthesized FeP/GA catalyst shows good electrocatalytic activity for HER in both acidic and alkaline solutions. The developed method can be useful for synthesizing metal hexacyanoferrate derived mono/bimetal phosphide catalyst in porous 3D graphene aerogels. 相似文献
11.
Jiayue Tian Feilong Jiang Daqiang Yuan Linjie Zhang Qihui Chen Maochun Hong 《Angewandte Chemie (International ed. in English)》2020,59(31):13101-13108
Facile preparation of low‐cost electrocatalysts for efficient oxygen evolution reaction (OER) remains a big challenge. Herein, a novel strategy for ultrafast (20 s) transformation of bulk metal–organic frameworks (MOFs) into ultrathin metal oxyhydroxide nanosheets for efficient OER has been developed. For two isomeric MOFs ( FJI‐H25Fe and FJI‐H25FeCo ), only the metastable FJI‐H25FeCo bulk can immediately transform into FeCo‐oxyhydroxides nanosheets through electric‐field assisted hydrolysis. The potential evolution process from MOF bulk to FeCo‐oxyhydroxides nanosheets has been investigated in detail. The as‐made nanosheets exhibit excellent OER performances, showing an extremely low overpotential of 231 mV at the current density of 10 mA cm?2, a relatively small Tafel slope of 42 mV dec?1, and long‐term durability of at least 30 h. This work not only provides a novel strategy for facile preparation of low‐cost and efficient OER electrocatalysts, but also represents a new way for preparation of metal oxyhydroxides nanosheets with good crystallinity and morphology, and a fresh method for mild synthesis of nanosized derivatives from MOF materials. 相似文献
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In this study, the electrochemical reduction of nitrite was investigated on poly(4‐aminoacetanilide) (PPAA) forming by cyclic voltammetry at the surface of carbon paste electrode. The electrochemical properties of the modified electrode have been studied by cyclic voltammetry and double potential step chronoamperometry. Results showed that in the optimum condition (pH = 0.00) the reduction of nitrite occurred at a potential about 667 mV more positive than that unmodified carbon paste electrode. This amount of electrocatalytic ability is high compared with other electrocatalysts. Using a chronoamperometric method, the catalytic rate constant (k) was calculated 8.4 × 104 cm3 mol‐1 s‐1. Also, the electrocatalytic reduction peak currents was found to be linear with the nitrite concentration in the ranges of 5 × 10‐4 M to 2.5 × 10‐2 M and 2 × 10‐5 M to 7 × 10‐3 M with detection limits (2σ) were determined as 4.5 × 10‐4 M and 1 × 10‐5 M by cyclic voltammetry (CV) and hydrodynamic amperometry methods respectively. Recovery experiments exhibit the satisfactory results. 相似文献
14.
Qiang Guo Jiaxing Dong Danyang Wan Di Wu Jingsong You 《Macromolecular rapid communications》2013,34(6):522-527
A concise, highly efficient palladium‐catalyzed direct C–H (hetero)arylation is developed to modularly assemble a diketopyrrolopyrrole ( DTDPP )‐based polymer library to screen low‐bandgap and near‐infrared (NIR) absorbing materials. The DTDPP ‐based copolymers P1 and P2 with an alternating donor–acceptor–donor–acceptor (D–A–D–A) sequence and the homopolymer P9 exhibit planarity and excellent π‐conjugation, which lead to low bandgaps (down to 1.22 eV) as well as strong and broad NIR absorption bands (up to 1000 nm). 相似文献
15.
A Reliable Aerosol‐Spray‐Assisted Approach to Produce and Optimize Amorphous Metal Oxide Catalysts for Electrochemical Water Splitting 下载免费PDF全文
Long Kuai Jing Geng Changyu Chen Erjie Kan Yadong Liu Qing Wang Prof. Dr. Baoyou Geng 《Angewandte Chemie (International ed. in English)》2014,53(29):7547-7551
An aerosol‐spray‐assisted approach (ASAA) is proposed and confirmed as a precisely controllable and continuous method to fabricate amorphous mixed metal oxides for electrochemical water splitting. The proportion of metal elements can be accurately controlled to within (5±5) %. The products can be sustainably obtained, which is highly suitable for industrial applications. ASAA was used to show that Fe6Ni10Ox is the best catalyst among the investigated Fe‐Ni‐Ox series with an overpotential of as low as 0.286 V (10 mA cm?2) and a Tafel slope of 48 mV/decade for the electrochemical oxygen evolution reaction. Therefore, this work contributes a versatile, continuous, and reliable way to produce and optimize amorphous metal oxide catalysts. 相似文献
16.
A Molecular Approach to Self‐Supported Cobalt‐Substituted ZnO Materials as Remarkably Stable Electrocatalysts for Water Oxidation 下载免费PDF全文
Johannes Pfrommer Dr. Michael Lublow Anahita Azarpira Dr. Caren Göbel Marcel Lücke Dr. Alexander Steigert Martin Pogrzeba Dr. Prashanth W. Menezes Dr. Anna Fischer Dr. Thomas Schedel‐Niedrig Prof. Dr. Matthias Driess 《Angewandte Chemie (International ed. in English)》2014,53(20):5183-5187
In regard to earth‐abundant cobalt water oxidation catalysts, very recent findings show the reorganization of the materials to amorphous active phases under catalytic conditions. To further understand this concept, a unique cobalt‐substituted crystalline zinc oxide (Co:ZnO) precatalyst has been synthesized by low‐temperature solvolysis of molecular heterobimetallic Co4?xZnxO4 (x=1–3) precursors in benzylamine. Its electrophoretic deposition onto fluorinated tin oxide electrodes leads after oxidative conditioning to an amorphous self‐supported water‐oxidation electrocatalyst, which was observed by HR‐TEM on FIB lamellas of the EPD layers. The Co‐rich hydroxide‐oxidic electrocatalyst performs at very low overpotentials (512 mV at pH 7; 330 mV at pH 12), while chronoamperometry shows a stable catalytic current over several hours. 相似文献
17.
Yuan Liu Xue Li Qinghua Zhang Weidong Li Yu Xie Hanyu Liu Lu Shang Zhongyi Liu Zhimin Chen Lin Gu Zhiyong Tang Tierui Zhang Siyu Lu 《Angewandte Chemie (International ed. in English)》2020,59(4):1718-1726
A challenging but pressing task to design and synthesize novel, efficient, and robust pH‐universal hydrogen evolution reaction (HER) electrocatalysts for scalable and sustainable hydrogen production through electrochemical water splitting. Herein, we report a facile method to prepare an efficient and robust Ru‐M (M=Ni, Mn, Cu) bimetal nanoparticle and carbon quantum dot hybrid (RuM/CQDs) for pH‐universal HER. The RuNi/CQDs catalysts exhibit outstanding HER performance at all pH levels. The unexpected low overpotentials of 13, 58, and 18 mV shown by RuNi/CQDs allow a current density of 10 mA cm?2 in 1 m KOH, 0.5 m H2SO4, and 1 m PBS, respectively, for Ru loading at 5.93 μgRu cm?2. This performance is among the best catalytic activities reported for any platinum‐free electrocatalyst. Theoretical studies reveal that Ni doping results in a moderate weakening of the hydrogen bonding energy of nearby surface Ru atoms, which plays a critical role in improving the HER activity. 相似文献
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Haixia Zhong Khoa Hoang Ly Mingchao Wang Yulia Krupskaya Xiaocang Han Jichao Zhang Jian Zhang Vladislav Kataev Bernd Büchner Inez M. Weidinger Stefan Kaskel Pan Liu Mingwei Chen Renhao Dong Xinliang Feng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(31):10787-10792
Layered two‐dimensional (2D) conjugated metal–organic frameworks (MOFs) represent a family of rising electrocatalysts for the oxygen reduction reaction (ORR), due to the controllable architectures, excellent electrical conductivity, and highly exposed well‐defined molecular active sites. Herein, we report a copper phthalocyanine based 2D conjugated MOF with square‐planar cobalt bis(dihydroxy) complexes (Co‐O4) as linkages (PcCu‐O8‐Co) and layer‐stacked structures prepared via solvothermal synthesis. PcCu‐O8‐Co 2D MOF mixed with carbon nanotubes exhibits excellent electrocatalytic ORR activity (E1/2=0.83 V vs. RHE, n=3.93, and jL=5.3 mA cm?2) in alkaline media, which is the record value among the reported intrinsic MOF electrocatalysts. Supported by in situ Raman spectro‐electrochemistry and theoretical modeling as well as contrast catalytic tests, we identified the cobalt nodes as ORR active sites. Furthermore, when employed as a cathode electrocatalyst for zinc–air batteries, PcCu‐O8‐Co delivers a maximum power density of 94 mW cm?2, outperforming the state‐of‐the‐art Pt/C electrocatalysts (78.3 mW cm?2). 相似文献