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1.
Defect Engineering Metal‐Free Polymeric Carbon Nitride Electrocatalyst for Effective Nitrogen Fixation under Ambient Conditions 下载免费PDF全文
Chade Lv Yumin Qian Chunshuang Yan Yu Ding Prof. Yuanyue Liu Prof. Gang Chen Prof. Guihua Yu 《Angewandte Chemie (International ed. in English)》2018,57(32):10246-10250
Electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions provides an intriguing picture for the conversion of N2 into NH3. However, electrocatalytic NRR mainly relies on metal‐based catalysts, and it remains a grand challenge in enabling effective N2 activation on metal‐free catalysts. Here we report a defect engineering strategy to realize effective NRR performance (NH3 yield: 8.09 μg h?1 mg?1cat., Faradaic efficiency: 11.59 %) on metal‐free polymeric carbon nitride (PCN) catalyst. Illustrated by density functional theory calculations, dinitrogen molecule can be chemisorbed on as‐engineered nitrogen vacancies of PCN through constructing a dinuclear end‐on bound structure for spatial electron transfer. Furthermore, the N?N bond length of adsorbed N2 increases dramatically, which corresponds to “strong activation” system to reduce N2 into NH3. This work also highlights the significance of defect engineering for improving electrocatalysts with weak N2 adsorption and activation ability. 相似文献
2.
Metal‐Substituted Zeolitic Imidazolate Framework ZIF‐108: Gas‐Sorption and Membrane‐Separation Properties 下载免费PDF全文
Yujie Ban Prof. Dr. Yanshuo Li Yuan Peng Hua Jin Wenmei Jiao Dr. Xinlei Liu Prof. Dr. Weishen Yang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2014,20(36):11402-11409
A series of dual‐metal zeolitic imidazolate framework (ZIF) crystals with SOD and RHO topologies was synthesised by metal substitution from ZIF‐108 (Zn(2‐nitroimidazolate)2, SOD topology) as the parent material. This was based on the concept that metal substitution of ZIF‐108 requires a much lower activation energy than homogenous nucleation owing to the metastability of ZIF‐108. In‐depth investigations of the formation processes of the daughter ZIFs indicated that the transformation of ZIF‐108 is a dissolution/heterogeneous nucleation process. Typical isostructural Co2+ substitution mainly occurs at the outer surface of ZIF‐108 and results in a core–shell structure. On the contrary, the Cu2+‐substituted ZIF has a RHO topology with a homogeneous distribution of Cu2+ ions in the structure. Substitution with Ni2+ resulted in a remarkable enhancement in adsorption selectivity toward CO2 over N2 by a factor of up to 227. With Co2+‐substituted nanoparticles as inorganic filler, a mixed matrix membrane based on polysulfone displayed greatly improved performance in the separation of H2/CH4, CO2/N2 and CO2/CH4. 相似文献
3.
Synthesis of N‐(1H‐imidazoline‐2‐yl)‐1H‐benzimidazol‐2‐amine was carried out under microwave irradiation (MWI) conditions. Dynamic 1H NMR investigation of N‐(1H‐imidazoline‐2‐yl)‐1H‐benzimidazol‐2‐amine compound was reported at temperature range of 223–333 K in DMF‐d7. Some physical parameters, such as coalescence temperature (Tc), the free energy of activation (ΔG??) and rate constant (k) values were calculated from its 1H NMR spectra at various temperatures. Electrochemical feature of this compound was investigated by cyclic (CV) and square wave voltammetry (SWV). 相似文献
4.
Teshica Chatturgoon Matthew P. Akerman 《Acta Crystallographica. Section C, Structural Chemistry》2016,72(3):234-238
The application of transition metal chelates as chemotherapeutic agents has the advantage that they can be used as a scaffold around which ligands with DNA recognition elements can be anchored. The facile substitution of these components allows for the DNA recognition and binding properties of the metal chelates to be tuned. Copper is a particularly interesting choice for the development of novel metallodrugs as it is an endogenous metal and is therefore less toxic than other transition metals. The title compound, [Cu(C16H11N2O)2], was synthesized by reacting N‐(quinolin‐8‐yl)benzamide and the metal in a 2:1 ratio. Ligand coordination required deprotonation of the amide N—H group and the isolated complex is therefore neutral. The metal ion adopts a flattened tetrahedral coordination geometry with the ligands in a pseudo‐trans configuration. The free rotation afforded by the formal single bond between the amide group and phenyl ring allows the phenyl rings to rotate out‐of‐plane, thus alleviating nonbonded repulsion between the phenyl rings and the quinolyl groups within the complex. Weak C—H…O interactions stabilize a dimer in the solid state. Density functional theory (DFT) simulations at the PBE/6‐311G(dp) level of theory show that the solid‐state structure (C1 symmetry) is 79.33 kJ mol−1 higher in energy than the lowest energy gas‐phase structure (C2 symmetry). Natural bond orbital (NBO) analysis offers an explanation for the formation of the C—H…O interactions in electrostatic terms, but the stabilizing effect is insufficient to support the dimer in the gas phase. 相似文献
5.
Synthesis of the First Example of the 12‐Vertex‐closo/12‐Vertex‐nido Biscarborane Cluster by a Metal‐Free B−H Activation at a Phosphorus(III) Center 下载免费PDF全文
Dr. Yuen Onn Wong Dr. Mark D. Smith Prof. Dmitry V. Peryshkov 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(20):6764-6767
An unusual 12‐vertex‐closo‐C2B10/12‐vertex‐nido‐C2B10 biscarborane cluster was synthesized through an unprecedented regioselective metal‐free B?H activation by a sterically hindered PIII center under mild conditions accompanied by cage‐opening rearrangement. A combination of the electron‐accepting properties of a carborane cage and steric enforcement of close interatomic contacts represent a new synthetic strategy for the activation of strong B?H bonds in carboranes. 相似文献
6.
Spectroscopic,DFT and antimicrobial activity of Zn(II), Zr(IV), Ce(IV) and U(VI) complexes of N,N‐ chelated 4,6‐bis (4‐chlorophenyl)‐2‐amino‐1,2‐dihydropyridine‐3‐carbinitrile 下载免费PDF全文
Four novel metal complexes of 4,6‐bis (4‐chlorophenyl)‐2‐amino‐1,2‐dihydropyridine‐3‐carbinitrile (H2L) with Zn(II), Zr(IV), Ce(IV) and U(VI) were synthesized. The structure was elucidated using elemental analysis, melting point, molar conductivity; spectroscopic techniques (IR, 1H NMR, UV–Vis., mass spectra) as well as thermo gravimetric analysis. The spectroscopic data proved that H2L chelated with the metal ions as a bidentate ligand through Namino and Ncarbinitrile atoms. The molecular structure of the complexes was determined using density functional theory (DFT). The central metal ion in each complex is six‐coordinate and the angles around it vary from 62.74° to 166.46°; these values agree with distorted octahedral geometry. The calculated total energy of the complexes found in the region – 406.342 to ?459.717 au and the dipole moment change from 4.675 to 13.171D. The antibacterial and antifungal activities of the ligand, metal salts and complexes were estimated on some microorganisms. The complexes showed significant antibacterial profile in comparison to the free ligand. 相似文献
7.
Yue Wang Miao‐miao Shi Di Bao Fan‐lu Meng Qi Zhang Yi‐tong Zhou Kai‐hua Liu Yan Zhang Jia‐zhi Wang Zhi‐wen Chen Da‐peng Liu Zheng Jiang Mi Luo Lin Gu Qing‐hua Zhang Xing‐zhong Cao Yao Yao Min‐hua Shao Yu Zhang Xin‐Bo Zhang Jingguang G. Chen Jun‐min Yan Qing Jiang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(28):9564-9569
The electrochemical N2 fixation, which is far from practical application in aqueous solution under ambient conditions, is extremely challenging and requires a rational design of electrocatalytic centers. We observed that bismuth (Bi) might be a promising candidate for this task because of its weak binding with H adatoms, which increases the selectivity and production rate. Furthermore, we successfully synthesized defect‐rich Bi nanoplates as an efficient noble‐metal‐free N2 reduction electrocatalyst via a low‐temperature plasma bombardment approach. When exclusively using 1H NMR measurements with N2 gas as a quantitative testing method, the defect‐rich Bi(110) nanoplates achieved a 15NH3 production rate of 5.453 μg mgBi?1 h?1 and a Faradaic efficiency of 11.68 % at ?0.6 V vs. RHE in aqueous solution at ambient conditions. 相似文献
8.
Li‐Na Wang Dr. Xiao‐Na Li Li‐Xue Jiang Bin Yang Dr. Qing‐Yu Liu Dr. Hong‐Guang Xu Prof. Wei‐Jun Zheng Prof. Sheng‐Gui He 《Angewandte Chemie (International ed. in English)》2018,57(13):3349-3353
Catalytic CO oxidation by molecular O2 is an important model reaction in both the condensed phase and gas‐phase studies. Available gas‐phase studies indicate that noble metal is indispensable in catalytic CO oxidation by O2 under thermal collision conditions. Herein, we identified the first example of noble‐metal‐free heteronuclear oxide cluster catalysts, the copper–vanadium bimetallic oxide clusters Cu2VO3–5? for CO oxidation by O2. The reactions were characterized by mass spectrometry, photoelectron spectroscopy, and density functional calculations. The dynamic nature of the Cu?Cu unit in terms of the electron storage and release is the driving force to promote CO oxidation and O2 activation during the catalysis. 相似文献
9.
Youwen Liu Ming Cheng Zhihai He Bingchuan Gu Chong Xiao Tengfei Zhou Zaiping Guo Jiandang Liu Haiyan He Bangjiao Ye Bicai Pan Yi Xie 《Angewandte Chemie (International ed. in English)》2019,58(3):731-735
Nitrate is a raw ingredient for the production of fertilizer, gunpowder, and explosives. Developing an alternative approach to activate the N≡N bond of naturally abundant nitrogen to form nitrate under ambient conditions will be of importance. Herein, pothole‐rich WO3 was used to catalyse the activation of N≡N covalent triple bonds for the direct nitrate synthesis at room temperature. The pothole‐rich structure endues the WO3 nanosheet more dangling bonds and more easily excited high momentum electrons, which overcome the two major bottlenecks in N≡N bond activation, that is, poor binding of N2 to catalytic materials and the high energy involved in this reaction. The average rate of nitrate production is as high as 1.92 mg g?1 h?1 under ambient conditions, without any sacrificial agent or precious‐metal co‐catalysts. More generally, the concepts will initiate a new pathway for triggering inert catalytic reactions. 相似文献
10.
Weiyan Ni Teng Wang Pascal Alexander Schouwink Yu‐Chun Chuang Hao Ming Chen Xile Hu 《Angewandte Chemie (International ed. in English)》2020,59(27):10797-10801
The hydroxide‐exchange membrane fuel cell (HEMFC) is a promising energy conversion device. However, the development of HEMFC is hampered by the lack of platinum‐group‐metal‐free (PGM‐free) electrocatalysts for the hydrogen oxidation reaction (HOR). Now, a Ni catalyst is reported that exhibits the highest mass activity in HOR for a PGM‐free catalyst as well as excellent activity in the hydrogen evolution reaction (HER). This catalyst, Ni‐H2‐2 %, was optimized through pyrolysis of a Ni‐containing metal‐organic framework precursor under a mixed N2/H2 atmosphere, which yielded carbon‐supported Ni nanoparticles with different levels of strains. The Ni‐H2‐2 % catalyst has an optimal level of strain, which leads to an optimal hydrogen binding energy and a high number of active sites. 相似文献
11.
Ting Wang Hong Ma Xin Liu Yang Luo Shujing Zhang Yuxia Sun Xinhong Wang Jin Gao Jie Xu 《化学:亚洲杂志》2019,14(9):1515-1522
It is an attractive and challenging topic to endow non‐noble metal catalysts with high efficiency via a nitrogen‐doping approach. In this study, a nitrogen‐doped carbon catalyst with high nitrogen content encapsulating cobalt NPs (CoOx@N‐C(g)) was synthesized, and characterized in detail by XRD, HRTEM, N2‐physisorption, ICP, CO2‐TPD, and XPS techniques. g‐C3N4 nanosheets act as nitrogen source and self‐sacrificing templates, giving rise to an ultrahigh nitrogen content of 14.0 %, much higher than those using bulk g‐C3N4 (4.4 %) via the same synthesis procedures. As a result, CoOx@N‐C(g) exhibited the highest performance in the oxidative esterification of biomass‐derived platform furfural to methylfuroate under base‐free conditions, achieving 95.0 % conversion and 97.1 % selectivity toward methylfuroate under 0.5 MPa O2 at 100 °C for 6 h, far exceeding those of other cobalt‐based catalysts. The high efficiency of CoOx@N‐C(g) was closely related to its high ratio of pyridinic nitrogen species that may act as Lewis basic sites as well as its capacity for the activation of dioxygen to superoxide radical O2.?. 相似文献
12.
Xiaoman Li Prof. Wenzhong Wang Dong Jiang Songmei Sun Ling Zhang Xiang Sun 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(39):13819-13822
Ammonia synthesis under mild conditions is of supreme interest. Photocatalytic nitrogen fixation with water at room temperature and atmospheric pressure is an intriguing strategy. However, the efficiency of this method has been far from satisfied for industrialization, mainly due to the sluggish cleavage of the N≡N bond. Herein, we report a carbon–tungstic‐acid (WO3 ? H2O) hybrid for the co‐optimization of N2 activation as well as subsequent photoinduced protonation. Efficient ammonia evolution reached 205 μmol g?1 h?1 over this hybrid under simulated sunlight. Nitrogen temperature‐programmed desorption revealed the decisive role of carbon in N2 adsorption. Photoactive WO3 ? H2O guaranteed the supply of electrons and protons for subsequent protonation. The universality of carbon modification for enhancing the N2 reduction was further verified over various photocatalysts, shedding light on future materials design for ideal solar energy utilization. 相似文献
13.
Leen E. E. Broeckx Sabriye Güven Frank J. L. Heutz Dr. Martin Lutz Prof. Dr. Dieter Vogt Prof. Dr. Christian Müller 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(39):13087-13098
A series of 2,4,6‐triarylphosphinines were prepared and investigated in the base‐assisted cyclometalation reaction using [Cp*IrCl2]2 (Cp*=1,2,3,4,5‐pentamethylcyclopentadienyl) as the metal precursor. Insight in the mechanism of the C? H bond activation of phosphinines as well as in the regioselectivity of the reaction was obtained by time‐dependent 31P{1H} NMR spectroscopy. At room temperature, 2,4,6‐triarylphosphinines instantaneously open the Ir‐dimer and coordinate in an η1‐fashion to the metal center. Upon heating, a dissociation step towards free ligand and an Ir‐acetate species is observed and proven to be a first‐order reaction with an activation energy of ΔEA=56.6 kJ mol?1 found for 2,4,6‐triphenylphosphinine. Electron‐donating substituents on the ortho‐phenyl groups of the phosphorus heterocycle facilitate the subsequent cyclometalation reaction, indicating an electrophilic C? H activation mechanism. The cyclometalation reaction turned out to be very sensitive to steric effects as even small substituents can have a large effect on the regioselectivity of the reaction. The cyclometalated products were characterized by means of NMR spectroscopy and in several cases by single‐crystal X‐ray diffraction. Based on the observed trends during the mechanistic investigation, a concerted base‐assisted metalation–deprotonation (CMD) mechanism, which is electrophilic in nature, is proposed. 相似文献
14.
Xiao‐Feng Wang Yangyang Chen Li‐Ping Song Zhen Fang Jian Zhang Fanian Shi Ying‐Wu Lin Yunkai Sun Yue‐Biao Zhang Joo Rocha 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(52):18984-18988
To efficiently capture the toxic uranyl ions (UO22+), a new hierarchical micro‐macroporous metal–organic framework was prepared under template‐free conditions, featuring interconnected multi‐nanocages bearing carbonyl groups derived from a semi‐rigid ligand. The material exhibits an unusually high UO22+ sorption capacity of 562 mg g?1, which occurs in an intriguing two‐steps process, on the macropore‐based crystal surface and in the inner nanocages. Notably, the latter is attributed to the cooperative interplay of the shrinkage of the host porous framework induced by uranyl accommodation and the free carbonyl coordination sites, as shown by both single‐crystal X‐ray diffraction and a red‐shift of the infrared [O=UVI=O]2+ antisymmetric vibration band. 相似文献
15.
Simon David Kloß Prof. Dr. Wolfgang Schnick 《Angewandte Chemie (International ed. in English)》2015,54(38):11250-11253
Developing a synthetic method to target an broad spectrum of unknown phases can lead to fascinating discoveries. The preparation of the first rare‐earth‐metal nitridophosphate LiNdP4N8 is reported. High‐pressure solid‐state metathesis between LiPN2 and NdF3 was employed to yield a highly crystalline product. The in situ formed LiF is believed to act both as the thermodynamic driving force and as a flux to aiding single‐crystal formation in dimensions suitable for crystal structure analysis. Magnetic properties stemming from Nd3+ ions were measured by SQUID magnetometry. LiNdP4N8 serves as a model system for the exploration of rare‐earth‐metal nitridophosphates that may even be expanded to transition metals. High‐pressure metathesis enables the systematic study of these uncharted regions of nitride‐based materials with unprecedented properties. 相似文献
16.
Ying Huang Bo Chen Jian Duan Fei Yang Tengrui Wang Zhengfeng Wang Wenjuan Yang Chenchen Hu Wei Luo Yunhui Huang 《Angewandte Chemie (International ed. in English)》2020,59(9):3699-3704
Solid‐state Li metal batteries (SSLMBs) have attracted considerable interests due to their promising energy density as well as high safety. However, the realization of a well‐matched Li metal/solid‐state electrolyte (SSE) interface remains challenging. Herein, we report g‐C3N4 as a new interface enabler. We discover that introducing g‐C3N4 into Li metal can not only convert the Li metal/garnet‐type SSE interface from point contact to intimate contact but also greatly enhance the capability to suppress the dendritic Li formation because of the greatly enhanced viscosity, decreased surface tension of molten Li, and the in situ formation of Li3N at the interface. Thus, the resulting Li‐C3N4|SSE|Li‐C3N4 symmetric cell gives a significantly low interfacial resistance of 11 Ω cm2 and a high critical current density (CCD) of 1500 μA cm?2. In contrast, the same symmetric cell configuration with pristine Li metal electrodes has a much larger interfacial resistance (428 Ω cm2) and a much lower CCD (50 μA cm?2). 相似文献
17.
An Amorphous Noble‐Metal‐Free Electrocatalyst that Enables Nitrogen Fixation under Ambient Conditions 下载免费PDF全文
Chade Lv Chunshuang Yan Prof. Gang Chen Yu Ding Dr. Jingxue Sun Yansong Zhou Prof. Guihua Yu 《Angewandte Chemie (International ed. in English)》2018,57(21):6073-6076
N2 fixation by the electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions is regarded as a potential approach to achieve NH3 production, which still heavily relies on the Haber–Bosch process at the cost of huge energy and massive production of CO2. A noble‐metal‐free Bi4V2O11/CeO2 hybrid with an amorphous phase (BVC‐A) is used as the cathode for electrocatalytic NRR. The amorphous Bi4V2O11 contains significant defects, which play a role as active sites. The CeO2 not only serves as a trigger to induce the amorphous structure, but also establishes band alignment with Bi4V2O11 for rapid interfacial charge transfer. Remarkably, BVC‐A shows outstanding electrocatalytic NRR performance with high average yield (NH3: 23.21 μg h?1 mg?1cat., Faradaic efficiency: 10.16 %) under ambient conditions, which is superior to the Bi4V2O11/CeO2 hybrid with crystalline phase (BVC‐C) counterpart. 相似文献
18.
Bis‐tert‐Alcohol‐Functionalized Crown‐6‐Calix[4]arene: An Organic Promoter for Nucleophilic Fluorination 下载免费PDF全文
Dr. Vinod H. Jadhav Wonsil Choi Sung‐Sik Lee Prof. Dr. Sungyul Lee Prof. Dr. Dong Wook Kim 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(13):4515-4520
A bis‐tert‐alcohol‐functionalized crown‐6‐calix[4]arene (BACCA) was designed and prepared as a multifunctional organic promoter for nucleophilic fluorinations with CsF. By formation of a CsF/BACCA complex, BACCA could release a significantly active and selective fluoride source for SN2 fluorination reactions. The origin of the promoting effects of BACCA was studied by quantum chemical methods. The role of BACCA was revealed to be separation of the metal fluoride to a large distance (>8 Å), thereby producing an essentially “free” F?. The synergistic actions of the crown‐6‐calix[4]arene subunit (whose O atoms coordinate the counter‐cation Cs+) and the terminal tert‐alcohol OH groups (forming controlled hydrogen bonds with F?) of BACCA led to tremendous efficiency in SN2 fluorination of base‐sensitive substrates. 相似文献
19.
Kristof Seubert Dominik Böhme Jutta Kösters Wei‐Zheng Shen Eva Freisinger Prof. Dr. Jens Müller 《无机化学与普通化学杂志》2012,638(11):1761-1767
Metal‐mediated base pairs can be used to insert metal ions into nucleic acids at precisely defined positions. As structural data on the resulting metal‐modified DNA are scarce, appropriate model complexes need to be synthesized and structurally characterized. Accordingly, the molecular structures of nine transition metal complexes of N‐methyl‐2, 2'‐dipicolylamine (dipic) are reported. In combination with an azole‐containing artificial nucleoside, this tridentate ligand had recently been used to generate metal‐mediated base pairs (Chem. Commun. 2011 , 47, 11041–11043). The PdII and PtII complexes reported here confirm that the formation of planar complexes (as required for a metal‐mediated base pair) comprising N‐methyl‐2, 2'‐dipicolylamine is possible. Two HgII complexes with differing stoichiometry indicate that a planar structure might also be formed with this metal ion, even though it is not favored. In the complex [Ag2(dipic)2](ClO4)2, the two AgI ions are located close to one another with an Ag ··· Ag distance of 2.9152(3) Å, suggesting the presence of a strong argentophilic interaction. 相似文献
20.
Rajendar Bandari Dr. Thomas Höche Dr. Andrea Prager Klaus Dirnberger Dr. Michael R. Buchmeiser Prof. Dr. 《Chemistry (Weinheim an der Bergstrasse, Germany)》2010,16(15):4650-4658
Monolithic polymeric supports have been prepared by electron‐beam‐triggered free‐radical polymerization using a mixture of glycidyl methacrylate and trimethylolpropane triacrylate in 2‐propanol, 1‐dodecanol, and toluene. Under appropriate conditions, phase separation occurred, which resulted in the formation of a porous monolithic matrix that was characterized by large (convective) pores in the 30 μm range as well as pores of <600 nm. The epoxy groups in pores of >7 nm were hydrolyzed by using poly(styrenesulfonic acid) (Mw=69 400 g mol?1, PDI=2.4). The remaining epoxy groups inside pores of <7 nm were subjected to aminolysis with norborn‐5‐en‐2‐ylmethylamine ( 2 ) and provided covalently bound norborn‐2‐ene (NBE) groups inside these pores. These NBE groups were then treated with the first‐generation Grubbs initiator [RuCl2(PCy3)2(CHPh)]. These immobilized Ru–alkylidenes were further used for the surface modification of the small pores by a grafting approach. A series of monomers, that is, 7‐oxanorborn‐5‐ene‐2,3‐dicarboxylic anhydride ( 3 ), norborn‐5‐ene‐2,3‐dicarboxylic anhydride ( 4 ), N,N‐di‐2‐pyridyl‐7‐oxanorborn‐5‐ene‐2‐carboxylic amide ( 5 ), N,N‐di‐2‐pyridylnorborn‐5‐ene‐2‐carboxamide ( 6 ), N‐[2‐(dimethylamino)ethyl]bicyclo[2.2.1]hept‐5‐ene‐2‐carboxamide ( 7 ), and dimethyl bicyclo[2.2.1]hept‐5‐en‐2‐ylphosphonate ( 8 ), were used for this purpose. Finally, monoliths functionalized with poly‐ 5 graft polymers were used to permanently immobilize Pd2+ and Pt4+, respectively, inside the pores. After reduction, metal nanoparticles 2 nm in diameter were formed. The palladium‐nanoparticle‐loaded monoliths were used in both Heck‐ and Suzuki‐type coupling reactions achieving turnover numbers of up to 167 000 and 63 000, respectively. 相似文献