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1.
Tuning the Adsorption Energy of Methanol Molecules Along Ni‐N‐Doped Carbon Phase Boundaries by the Mott–Schottky Effect for Gas‐Phase Methanol Dehydrogenation
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Zhong‐Hua Xue Jing‐Tan Han Wei‐Jie Feng Qiu‐Ying Yu Prof. Xin‐Hao Li Prof. Markus Antonietti Prof. Jie‐Sheng Chen 《Angewandte Chemie (International ed. in English)》2018,57(10):2697-2701
Engineering the adsorption of molecules on active sites is an integral and challenging part for the design of highly efficient transition‐metal‐based catalysts for methanol dehydrogenation. A Mott–Schottky catalyst composed of Ni nanoparticles and tailorable nitrogen‐doped carbon‐foam (Ni/NCF) and thus tunable adsorption energy is presented for highly efficient and selective dehydrogenation of gas‐phase methanol to hydrogen and CO even under relatively high weight hourly space velocities (WHSV). Both theoretical and experimental results reveal the key role of the rectifying contact at the Ni/NCF boundaries in tailoring the electron density of Ni species and enhancing the absorption energies of methanol molecules, which leads to a remarkably high turnover frequency (TOF) value (356 mol methanol mol?1 Ni h?1 at 350 °C), outpacing previously reported bench‐marked transition‐metal catalysts 10‐fold. 相似文献
2.
Alexander K. Tucker‐Schwartz Prof. Dr. Robin L. Garrell 《Chemistry (Weinheim an der Bergstrasse, Germany)》2010,16(42):12718-12726
The organic oxidant TEMPO (2,2,4,4‐tetramethylpiperdine‐1‐oxyl) was immobilized on iron oxide (Fe3O4) superparamagnetic nanoparticles by employing strong metal‐oxide chelating phosphonates and azide/alkyne “click” chemistry. This simple preparation yields recyclable TEMPO‐coated nanoparticles with good TEMPO loadings. They have excellent magnetic response and efficiently catalyze the oxidation of a wide range of primary and secondary alcohols to aldehydes, ketones, and lactones under either aerobic acidic MnII/CuII oxidizing Minisci conditions, or basic NaOCl Anelli conditions. The nanoparticles could be recycled more than 20 times under the Minisci conditions and up to eight times under the Anelli conditions with good to excellent substrate conversions and product selectivities. Immobilization of the catalyst through a phosphonate linkage allows the particles to withstand acidic oxidizing environments with minimal catalyst leaching. Clicking TEMPO to the phosphonate prior to phosphonate immobilization, rather than after, ensures the clicked catalyst is the only species on the particle surface. This facilitates quantification of the catalyst loading. The stability of the phosphonate linker and simplicity of this catalyst immobilization method make this an attractive approach for tethering catalysts to oxide supports, creating magnetically separable catalysts that can be used under neutral or acidic conditions. 相似文献
3.
Dr. Renat Kadyrov 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(3):1002-1012
An efficient procedure is described for ring‐closing metathesis reactions. A conversion of 95 % for diethyl diallylmalonate in dilute solution could be achieved within a few minutes, reaching TOF=4173 min?1, with very low loading of commercially available Ru catalysts that contained unsaturated NHC ligands. In general, only 50 to 250 ppm of the catalyst is required to achieve near‐quantitative conversion into a broad variety of 5–16‐membered heterocyclic compounds. The practicality of this procedure was illustrated in the synthesis of 5–8‐membered N‐tert‐butoxycarbonyl (N‐Boc)‐ and N‐para‐toluenesulfonyl (N‐Ts)‐protected cyclic amines and 9–16‐membered lactones. The synthesis of macrocyclic proline‐based lactams required slightly higher catalyst loadings. Along with monocyclic products, oligomeric byproducts, mostly cyclodimers, were isolated and characterized. 相似文献
4.
Zhi Cai Lidong Li Youwei Zhang Zhao Yang Jie Yang Yingjie Guo Lin Guo 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(13):4233-4238
Electrochemical water splitting requires efficient, low‐cost water oxidation catalysts to accelerate the sluggish kinetics of the water oxidation reaction. A rapid photocorrosion method is now used to synthesize the homogeneous amorphous nanocages of Cu‐Ni‐Fe hydr(oxy)oxide as a highly efficient electrocatalyst for the oxygen evolution reaction (OER). The as‐fabricated product exhibits a low overpotential of 224 mV on a glassy carbon electrode at 10 mA cm?2 (even lower down to 181 mV when supported on Ni foam) with a Tafel slope of 44 mV dec?1 for OER in an alkaline solution. The obtained catalyst shows an extraordinarily large mass activity of 1464.5 A g?1 at overpotential of 300 mV, which is the highest mass activity for OER. This synthetic strategy may open a brand new pathway to prepare copper‐based ternary amorphous nanocages for greatly enhanced oxygen evolution. 相似文献
5.
Axial base‐controlled catalytic activity,oxidative stability and product selectivity of water‐insoluble manganese and iron porphyrins for oxidation of styrenes in water under green conditions
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A series of water‐insoluble iron(III) and manganese(III) porphyrins, FeT(2‐CH3)PPCl, FeT(4‐OCH3)PPCl, FeT(2‐Cl)PPCl, FeTPPCl, MnT(2‐CH3)PPOAc, MnT(4‐OCH3)PPOAc, MnT(2‐Cl)PPOAc and MnTPPOAc, in the presence of imidazole (ImH), F?, Cl?, Br? and acetate were used as catalysts for the aqueous‐phase heterogeneous oxidation of styrenes to the corresponding epoxides and aldehydes with sodium periodate. Also, the effect of various reaction parameters such as reaction time, molar ratio of catalyst to axial base, type of axial base, molar ratio of olefin to oxidant and nature of metal centre on the activity and oxidative stability of the catalysts and the product selectivity was investigated. Higher catalytic activities were found for the iron complexes. Interestingly, the selectivity towards the formation of epoxide and aldehyde (or acetophenone) was significantly influenced by the type of axial base. Furthermore, Br? and ImH were found to be the most efficient co‐catalysts for the oxidation of olefins performed in the presence of the manganese and iron porphyrins, respectively. The optimized molar ratio of catalyst to axial base was different for various axial bases. Also, the order of co‐catalyst activity of the axial bases obtained in aqueous medium was different from that reported for organic solvents. The use of a convenient axial base under optimum reaction catalyst to co‐catalyst molar ratio in the presence of the manganese porphyrin gave the oxidative products with a conversion of ca 100% in a reaction time of less than 3 h. However, the catalytic activity of the iron porphyrins could not be effectively improved by increasing the catalyst to co‐catalyst molar ratio. 相似文献
6.
Dr. Kuan‐Ting Lee Dai‐Ming Liu Prof. Shih‐Yuan Lu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(31):10877-10883
SnFe2O4 nanocrystals (NC), prepared with a simple one‐step carrier‐solvent‐assisted interfacial reaction process, were developed as highly efficient catalysts for hydrogen peroxide sensing. These NCs, with a size of around 7 nm, served as the sensing catalyst and were decorated onto the pore surfaces of a porous fluorine‐doped tin oxide (PFTO) host electrode, prepared from commercial FTO glass with a simple anodic treatment, to form the sensing electrode for hydrogen peroxide. The SnFe2O4 NCs‐loaded PFTO electrode exhibited an ultra‐high sensitivity of 1027 mA m ?1 cm?2 toward hydrogen peroxide, outperforming Pt NCs‐loaded PFTO electrodes. The SnFe2O4 NCs‐loaded PFTO electrode proved a promising relatively low cost, high performance sensing electrode for hydrogen peroxide. 相似文献
7.
Electro‐assembly of a Chromophore–Catalyst Bilayer for Water Oxidation and Photocatalytic Water Splitting
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Dr. Dennis L. Ashford Dr. Benjamin D. Sherman Dr. Robert A. Binstead Prof. Joseph L. Templeton Prof. Thomas J. Meyer 《Angewandte Chemie (International ed. in English)》2015,54(16):4778-4781
The use of electropolymerization to prepare electrocatalytically and photocatalytically active electrodes for water oxidation is described. Electropolymerization of the catalyst RuII(bda)(4‐vinylpyridine)2 (bda=2,2′‐bipyridine‐6,6′‐dicarboxylate) on planar electrodes results in films containing semirigid polymer networks. In these films there is a change in the water oxidation mechanism compared to the solution analogue from bimolecular to single‐site. Electro‐assembly construction of a chromophore–catalyst structure on mesoporous, nanoparticle TiO2 films provides the basis for a dye‐sensitized photoelectrosynthesis cell (DSPEC) for sustained water splitting in a pH 7 phosphate buffer solution. Photogenerated oxygen was measured in real‐time by use of a two‐electrode cell design. 相似文献
8.
A series of neutral binuclear iridium and rhodium complexes were synthesized based on bis‐imine ligands under mild conditions. These half‐sandwich late transition metal complexes were isolated in good yields and characterized by elemental analysis, 1H NMR, 13C NMR, HR‐MS, and FT‐IR spectroscopies, and the solid state structure of complexes 1 and 2 were further confirmed by single‐crystal X‐ray diffraction. Cyclic voltammetry (CV) characterization indicated that the complex 1 has the best catalyst for water oxidation process with TOF of 0.8 s?1 at low overpotential of 0.325 V in methanol‐phosphate buffer. The proposed double‐site water oxidation mechanism had been also speculated . 相似文献
9.
Ren Hommelsheim Yujing Guo Zhen Yang Claire Empel Rene M. Koenigs 《Angewandte Chemie (International ed. in English)》2019,58(4):1203-1207
Carbenes are very important reactive intermediates to access a variety of complex molecules and are applied widely in organic synthesis and drug discovery. Typically, their chemistry is accessed by the use of transition metal catalysts. Herein, we describe the application of low‐energy blue light for the photochemical generation of carbenes from donor–acceptor diazoalkanes. This catalyst‐free and operationally simple approach enables highly efficient cyclopropenation reactions with alkynes and the rearrangement of sulfides under mild reaction conditions, which can be utilized for both batch and continuous‐flow processes. 相似文献
10.
Dr. Xiangheng Niu Prof. Dr. Minbo Lan Dr. Hongli Zhao Dr. Chen Chen 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(29):9534-9541
The investigation of highly efficient catalysts for the electrochemical oxidation of glucose is the most critical challenge to commercialize nonenzymatic glucose sensors, which display a few attractive superiorities including the sufficient stability of their properties and the desired reproducibility of results over enzyme electrodes. Herein we propose a new and very promising catalyst: Pt cubes well‐dispersed on the porous Cu foam, for the the electrochemical oxidation reaction of glucose in neutral media. The catalyst is fabricated in situ on a homemade screen‐printed carbon electrode (SPCE) substrate through initially synthesizing the three‐dimensional (3D) porous Cu foam using a hydrogen evolution assisted electrodeposition strategy, followed by electrochemically reducing the platinic precursor simply and conveniently. Field emission scanning electron microscopy (FESEM) and transmission electron microscopy (TEM) proofs demonstrate that Pt cubes, with an average size (the distance of opposite faces) of 185.1 nm, highly dispersed on the macro/nanopore integrated Cu foam support can be reproducibly obtained. The results of electrochemical tests indicate that the cubic Pt‐based catalyst exhibits significant enhancement on the catalytic activity towards the electrooxidation of glucose in the presence of chloride ions, providing a specific activity 6.7 times and a mass activity 5.3 times those of commercial Pt/C catalysts at ?0.4 V (vs. Ag/AgCl). In addition, the proposed catalyst shows excellent stability of performance, with only a 2.8 % loss of electrocatalytic activity after 100 repetitive measurements. 相似文献
11.
Lei Shi Xingwang Wang Dr. Christian A. Sandoval Prof. Dr. Zheng Wang Prof. Dr. Hongji Li Jiang Wu Liting Yu Kuiling Ding Prof. Dr. 《Chemistry (Weinheim an der Bergstrasse, Germany)》2009,15(38):9855-9867
Well‐designed, self‐assembled, metal–organic frameworks were constructed by simple mixing of multitopic MonoPhos‐based ligands ( 3 ; MonoPhos=chiral, monodentate phosphoramidites based on the 1,1′‐bi‐2‐naphthol platform) and [Rh(cod)2]BF4 (cod=cycloocta‐1,5‐diene). This self‐supporting strategy allowed for simple and efficient catalyst immobilization without the use of extra added support, giving well‐characterized, insoluble (in toluene) polymeric materials ( 4 ). The resulting self‐supported catalysts ( 4 ) showed outstanding catalytic performance for the asymmetric hydrogenation of a number of α‐dehydroamino acids ( 5 ) and 2‐aryl enamides ( 7 ) with enantiomeric excess (ee) ranges of 94–98 % and 90–98 %, respectively. The linker moiety in 4 influenced the reactivity significantly, albeit with slight impact on the enantioselectivity. Acquisition of reaction profiles under steady‐state conditions showed 4 h and 4 i to have the highest reactivity (turnover frequency (TOF)=95 and 97 h?1 at 2 atm, respectively), whereas appropriate substrate/catalyst matching was needed for optimum chiral induction. The former was recycled 10 times without loss in ee (95–96 %), although a drop in TOF of approximately 20 % per cycle was observed. The estimation of effective catalytic sites in self‐supported catalyst 4 e was also carried out by isolation and hydrogenation of catalyst–substrate complex, showing about 37 % of the RhI centers in the self‐supported catalyst 4 e are accessible to substrate 5 c in the catalysis. A continuous flow reaction system using an activated C/ 4 h mixture as stationary‐phase catalyst for the asymmetric hydrogenation of 5 b was developed and run continuously for a total of 144 h with >99 % conversion and 96–97 % enantioselectivity. The total Rh leaching in the product solution is 1.7 % of that in original catalyst 4 h . 相似文献
12.
Nanosized IrOx–Ir Catalyst with Relevant Activity for Anodes of Proton Exchange Membrane Electrolysis Produced by a Cost‐Effective Procedure
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Philipp Lettenmeier Li Wang Dr. Ute Golla‐Schindler Dr. Pawel Gazdzicki Natalia A. Cañas Michael Handl Prof. Dr. Renate Hiesgen Dr. Seyed S. Hosseiny Dr. Aldo S. Gago Prof. Dr. Kaspar A. Friedrich 《Angewandte Chemie (International ed. in English)》2016,55(2):742-746
We have developed a highly active nanostructured iridium catalyst for anodes of proton exchange membrane (PEM) electrolysis. Clusters of nanosized crystallites are obtained by reducing surfactant‐stabilized IrCl3 in water‐free conditions. The catalyst shows a five‐fold higher activity towards oxygen evolution reaction (OER) than commercial Ir‐black. The improved kinetics of the catalyst are reflected in the high performance of the PEM electrolyzer (1 mgIr cm?2), showing an unparalleled low overpotential and negligible degradation. Our results demonstrate that this enhancement cannot be only attributed to increased surface area, but rather to the ligand effect and low coordinate sites resulting in a high turnover frequency (TOF). The catalyst developed herein sets a benchmark and a strategy for the development of ultra‐low loading catalyst layers for PEM electrolysis. 相似文献
13.
Iridium‐Catalyst‐Based Autonomous Bubble‐Propelled Graphene Micromotors with Ultralow Catalyst Loading
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Hong Wang Dr. Zdeněk Sofer Alex Yong Sheng Eng Prof. Martin Pumera 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(46):14946-14950
A novel concept of an iridium‐based bubble‐propelled Janus‐particle‐type graphene micromotor with very high surface area and with very low catalyst loading is described. The low loading of Ir catalyst (0.54 at %) allows for fast motion of graphene microparticles with high surface area of 316.2 m2 g?1. The micromotor was prepared with a simple and scalable method by thermal exfoliation of iridium‐doped graphite oxide precursor composite in hydrogen atmosphere. Oxygen bubbles generated from the decomposition of hydrogen peroxide at the iridium catalytic sites provide robust propulsion thrust for the graphene micromotor. The high surface area and low iridium catalyst loading of the bubble‐propelled graphene motors offer great possibilities for dramatically enhanced cargo delivery. 相似文献
14.
Dr. Zaifang Li Guoqiang Ma Ru Ge Fei Qin Xinyun Dong Wei Meng Tiefeng Liu Jinhui Tong Fangyuan Jiang Yifeng Zhou Ke Li Xue Min Prof. Dr. Kaifu Huo Prof. Dr. Yinhua Zhou 《Angewandte Chemie (International ed. in English)》2016,55(3):979-982
Thick, uniform, easily processed, highly conductive polymer films are desirable as electrodes for solar cells as well as polymer capacitors. Here, a novel scalable strategy is developed to prepare highly conductive thick poly(3,4‐ethylenedioxythiophene):polystyrene sulfonate (HCT‐PEDOT:PSS) films with layered structure that display a conductivity of 1400 S cm?1 and a low sheet resistance of 0.59 ohm sq?1. Organic solar cells with laminated HCT‐PEDOT:PSS exhibit a performance comparable to the reference devices with vacuum‐deposited Ag top electrodes. More importantly, the HCT‐PEDOT:PSS film delivers a specific capacitance of 120 F g?1 at a current density of 0.4 A g?1. All‐solid‐state flexible symmetric supercapacitors with the HCT‐PEDOT:PSS films display a high volumetric energy density of 6.80 mWh cm?3 at a power density of 100 mW cm?3 and 3.15 mWh cm?3 at a very high power density of 16160 mW cm?3 that outperforms previous reported solid‐state supercapacitors based on PEDOT materials. 相似文献
15.
《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(47):15149-15153
Flow batteries (FBs) are one of the most promising stationary energy‐storage devices for storing renewable energy. However, commercial progress of FBs is limited by their high cost and low energy density. A neutral zinc–iron FB with very low cost and high energy density is presented. By using highly soluble FeCl2/ZnBr2 species, a charge energy density of 56.30 Wh L−1 can be achieved. DFT calculations demonstrated that glycine can combine with iron to suppress hydrolysis and crossover of Fe3+/Fe2+. The results indicated that an energy efficiency of 86.66 % can be obtained at 40 mA cm−2 and the battery can run stably for more than 100 cycles. Furthermore, a low‐cost porous membrane was employed to lower the capital cost to less than $ 50 per kWh, which was the lowest value that has ever been reported. Combining the features of low cost, high energy density and high energy efficiency, the neutral zinc–iron FB is a promising candidate for stationary energy‐storage applications. 相似文献
16.
N. Kritchayanon N. Thanabodeekij S. Jitkarnka A. M. Jamieson S. Wongkasemjit 《应用有机金属化学》2006,20(2):155-160
Fe‐MFI zeolite was successfully synthesized using silatrane as precursor and tetrapropyl ammonium bromide as template via the sol–gel process and microwave heating technique. The effects of ageing time, heating temperature, heating time and iron concentration were investigated, and it was found that Fe‐MFI synthesis favors higher heating temperatures, but is limited by the degradation of the incorporation of a template molecule. Moreover, longer ageing and heating times promote the incorporation of higher amounts of iron atom in the MFI structure. However, too long an ageing time decreases the incorporation of iron. The lower the percentage Fe loading, the greater the percentage of Fe3+ ions incorporated into the MFI framework. The catalytic activity of Fe‐MFI catalyst for the oxidation of CO was studied and it was found that these synthesized catalysts catalyzed the oxidation of CO very well. Copyright © 2005 John Wiley & Sons, Ltd. 相似文献
17.
Evaluation of Fe and Ru Pincer‐Type Complexes as Catalysts for the Racemization of Secondary Benzylic Alcohols
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Dr. Oscar Verho Prof. Dr. Matthias Beller Prof. Dr. Jan‐E. Bäckvall 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(33):11583-11586
Fe and Ru pincer‐type catalysts are used for the racemization of benzylic alcohols. Racemization with the Fe catalyst was achieved within 30 minutes under mild reaction conditions, with a catalyst loading as low as 2 mol %. This reaction constitutes the first example of an iron‐catalyzed racemization of an alcohol. The efficiency for racemization of the Fe catalyst and its Ru analogue was evaluated for a wide range of sec‐benzylic alcohols. The commercially available Ru complex proved to be highly robust and even tolerated the presence of water in the reaction mixture. 相似文献
18.
《化学:亚洲杂志》2017,12(10):1095-1103
The synthesis of solid catalysts for the co‐catalyst‐free cycloaddition of CO2 has attracted much attention. Herein, we report a hierarchical porous organic polymer, Py‐Zn@MA, that is able to catalyze the cycloaddition reaction of epoxides and CO2 without using any additives or co‐catalyst to afford turnover frequency (TOF) values as high as 250 and 97 h−1 at 130 °C by using pure and diluted CO2 (simulating flue gas), respectively. These results are superior to those obtained from previously reported heterogeneous co‐catalyst‐free systems. The high activity of Py‐Zn@MA is mainly attributed to its bifunctional nature with ZnBr2 and pyridine activating the epoxide in a cooperative way. Notably, Py‐Zn@MA can be easily prepared on a large scale without using any catalyst and the chemicals are cost effective. Moreover, Py‐Zn@MA shows good substrate universality for the cycloaddition reactions of epoxides. Our designed porous organic polymer Py‐Zn@MA material has the potential to serve as an efficient catalyst for the direct conversion of flue gas with epoxides into value‐added cyclic carbonates. 相似文献
19.
Heterogeneous Catalysis for Water Oxidation by an Iridium Complex Immobilized on Bipyridine‐Periodic Mesoporous Organosilica
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Dr. Xiao Liu Yoshifumi Maegawa Dr. Yasutomo Goto Prof. Kenji Hara Dr. Shinji Inagaki 《Angewandte Chemie (International ed. in English)》2016,55(28):7943-7947
Heterogenization of metal‐complex catalysts for water oxidation without loss of their catalytic activity is important for the development of devices simulating photosynthesis. In this study, efficient heterogeneous iridium complexes for water oxidation were prepared using bipyridine‐bridged periodic mesoporous organosilica (BPy‐PMO) as a solid chelating ligand. The BPy‐PMO‐based iridium catalysts (Ir‐BPy‐PMO) were prepared by postsynthetic metalation of BPy‐PMO and characterized through physicochemical analyses. The Ir‐BPy‐PMOs showed high catalytic activity for water oxidation. The turnover frequency (TOF) values for Ir‐BPy‐PMOs were one order of magnitude higher than those of conventional heterogeneous iridium catalysts. The reusability and stability of Ir‐BPy‐PMO were also examined, and detailed characterization was conducted using powder X‐ray diffraction, nitrogen adsorption, 13C DD MAS NMR spectroscopy, TEM, and XAFS methods. 相似文献
20.
《化学:亚洲杂志》2017,12(5):543-551
Vertically aligned Ni(OH)2 nanosheets were grown on carbon paper (CP) current collectors through a simple and cost‐effective hydrothermal approach. The as‐grown nanosheets are porous and highly crystallized. If used as a monolithic electrode for electrochemical water oxidation in alkaline solution, the carbon paper supported Ni(OH)2 nanosheets [CP@Ni(OH)2] exhibit high electrocatalytic activity and excellent long‐term stability. The electrode can attain an anodic current density of 20 mA cm−2 at a low overpotential of 338 mV, comparable to that of state‐of‐the‐art RuO2 nanocatalysts supported on CP (CP/RuO2) with the same catalyst loading. Significantly, CP@Ni(OH)2 shows much better long‐term stability than CP/RuO2 upon continuous galvanostatic electrolysis, particularly at a high industry‐relevant current density such as 100 mA cm−2. CP@Ni(OH)2 can sustain water oxidation at 100 mA cm−2 for 50 h without any degradation, whereas the performance of CP/RuO2 is much poorer and deteriorates gradually over time. CP@Ni(OH)2 electrodes hold substantial promise for use as low‐costing water oxidation anodes in electrolyzers. 相似文献