We report a facile electroless chemical deposition(ECD)method to deposit uniform Pd nanoparticles((2.5±0.6)nm)on CeO2 nanorods(PdNPs/CeO2-ECD)through the interface redox reaction between the reduced CeO2 and Na2P...We report a facile electroless chemical deposition(ECD)method to deposit uniform Pd nanoparticles((2.5±0.6)nm)on CeO2 nanorods(PdNPs/CeO2-ECD)through the interface redox reaction between the reduced CeO2 and Na2PdCl4.Pd NPs/CeO2-ECD exhibits a stronger electronic metal-support interaction(EMSI)evidenced by higher reducibility and stronger anti-sintering capability at high temperatures,compared to that prepared by the conventional impregnation method.Such an EMSI effect of PdNPs/CeO2-ECD significantly improves its catalytic activity in CO oxidation.Besides,the chlorine residue-free catalysts through ECD process avoid the deleterious effect of chlorine on CO oxidation.This ECD process can further be extended to deposit various uniform nanoscaled noble metals(Au,Ag,Pt,Ru,Rh,etc.)on CeO2,which may deliver their potentials in advanced catalysis.展开更多
Cobalt carbide has recently been reported to catalyse the FTO con version of syngas with high selectivity for the production of lower olefins (C2-C4). Clarifying the formation process and atomic structure of cobalt ca...Cobalt carbide has recently been reported to catalyse the FTO con version of syngas with high selectivity for the production of lower olefins (C2-C4). Clarifying the formation process and atomic structure of cobalt carbide will help understand the catalytic mechanism of FTO. Herein, hydrogenati on of carb on monoxide was investigated for cobalt carbide synthesized from CoMn catalyst, followed by X-ray diffraction, transmission electron microscopy, temperature programmed reaction and in situ X-ray absorption spectroscopy. By monitoring the evolution of cobalt carbide during syngas conversion, the wavelet transform results give evidenee for the formation of the cobalt carbide and clearly demonstrate that the active site of catalysis was cobalt carbide.展开更多
Cobalt carbide(Co2C)was considered as potential catalysts available for large-scale industrialization of transforming syngas(H2 and CO)to clean fuels.Herein,we successfully synthesized Co-based catalysts with MnO supp...Cobalt carbide(Co2C)was considered as potential catalysts available for large-scale industrialization of transforming syngas(H2 and CO)to clean fuels.Herein,we successfully synthesized Co-based catalysts with MnO supported,to comprehend the effects of Co2C for Fischer–Tropsch synthesis(FTS)under ambient conditions.The huge variety of product selectivity which was contained by different active sites(Co and Co2C)has been found.Furthermore,density functional theory(DFT)shows that Co2C is efficacious of CO adsorption,whereas is weaker for H adsorption than Co.Combining the advantages of Co and Co2C,the catalyst herein can not only obtain more C5+products but also suppress methane selectivity.It can be a commendable guide for the design of industrial application products in FTS.展开更多
Herein,we prepared a bimetallic layered double hydroxide(FeCo LDH)featuring a dandelion-like structure.Anchoring of CeO_(2)onto FeCo LDH produced interfaces between the functionalizing CeO_(2)and the parent LDH.Compar...Herein,we prepared a bimetallic layered double hydroxide(FeCo LDH)featuring a dandelion-like structure.Anchoring of CeO_(2)onto FeCo LDH produced interfaces between the functionalizing CeO_(2)and the parent LDH.Comparative electrochemical studies were carried out.Onset potential,overpotential,and Tafel slope point to the superior oxygen-evolving performance of CeO_(2)-FeCo LDH with respect to FeCo LDH,therefore,demonstrating the merits of CeO_(2)functionalization.The electronic structures of Fe,Co,and Ce were analyzed by X-ray photoelectron spectroscopy(XPS)and electron energy loss spectroscopy(EELS)from which the increase of Co^(3+)and the concurrent lowering of Ce^(4+)were established.With the use of CeO_(2)-FeCo LDH,accelerated formation at a sizably reduced potential of Co-OOH,one of the key intermediates preceding the release of O_(2)was observed by in situ Raman spectroscopy.We now have the atomic-level and location-specific evidence,the increase of the active Co^(3+)across the interface to correlate the enhanced catalytic performance with CeO_(2)functionalization.展开更多
The strategy of element substitution is an effective way to tune the electronic structures of the active sites in catalysts, thereby leading to improvements in both the catalytic activity and stability. Herein, we des...The strategy of element substitution is an effective way to tune the electronic structures of the active sites in catalysts, thereby leading to improvements in both the catalytic activity and stability. Herein, we design and synthesize pyrite-type nickel/phosphorus co-doped CoS2 nanowires on carbon cloth （NiCoPS/CC） as efficient and durable electrodes for water electrolysis. Introduction of nickel and phosphorus produced stepwise and superb enhancement of the performance of the electrodes in the hydrogen evolution reaction due to regulation of the electronic structures of the active sites of the catalyst and accelerated charge transfer over a wide pH range （0-14）. The NiCoPS/CC electrodes also delivered a nearly undecayed catalytic current density of 10 mA.cm-2 at a low overpotential of 230 mV for oxygen evolution due to in situ formation of surficial Ni-Co oxo/hydroxide in 1.0 M KOH. Thus, the NiCoPS/CC electrodes gave rise to a catalytic current density of 10 mA·cm-2 for overall water splitting at potentials as low as 1.54 V during operation over 100 h in 1.0 M KOH with a Faradic efficiency of ~100%.展开更多
Silicon-based electrodes have attracted great attention in the artificial photosynthetic systems that mimic natural photosynthesis and directly convert the solar energy into chemical energy. Despite significant effort...Silicon-based electrodes have attracted great attention in the artificial photosynthetic systems that mimic natural photosynthesis and directly convert the solar energy into chemical energy. Despite significant efforts to date,catalytic stability of the silicon photoelectrodes is limited by their poor electrochemical stability. The formation of passivation or protective layers provides a feasible strategy to improve the photocatalytic stability of silicon photoelectrodes. Many candidates including metals, metal oxides, metal silicides and polymers have been explored as the protection layers for silicon photoelectrodes. The present review gives a concise overview of the protected silicon photoanodes for water oxidation with a focus on the relationship between the structural architecture of silicon photoanodes and their photocatalytic activity and stability.展开更多
To further investigate the influence of metal ions on the allylic rearrangement of 3,4,5,6-tetrahydrophthalic an- hydride during the hydrothermal reaction, metal ions such as manganese（Ⅱ）, zinc（Ⅱ） and cadmium（...To further investigate the influence of metal ions on the allylic rearrangement of 3,4,5,6-tetrahydrophthalic an- hydride during the hydrothermal reaction, metal ions such as manganese（Ⅱ）, zinc（Ⅱ） and cadmium（Ⅱ） have been employed in the synthesis, which leads to the formation of three new lamellar coordination polymers, [MnⅡs（μ3-OH）3（1-chec）（1,2-chedc）（2,3-chedc）2（H20）] （3Mn）, [ZnⅡs（μ3-OH）3（1-chec）（1,2-chedc）（2,3-chedc）2（H20）] （4Zn）, and [CdⅡ3（μ3-OH）2（1,2-chedc）2] （5Cd） （1-chec=cyclohexene-l-carboxylate, 1,2-chedc=cyclohexene-1,2- dicarboxylate, 2,3-chedc=cyclohexene-1,2-dicarboxylate）. Interestingly, the allylic rearrangement reaction is metal-dependent, which occurs only in 3Mn and 4Zn, resulting in the formation of one chiral carbon atom of the corresponding dicarboxylate ligands in both compounds. In addition, the magnetic property of compound 3Mn was studied, which revealed strong antiferromagnetic interactions between the metal centers.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.21872109 and 61774109)the State Key Laboratory for Mechanical Behavior of Materials(No.20182005)+3 种基金the Hundred Talents Program of Shanxi Provincethe Youth"Sanjin"Scholar Programthe Key R&D Project of Shanxi Province(No.201603D421032)supported by the Cyrus Tang Foundation through Tang Scholar Program。
文摘We report a facile electroless chemical deposition(ECD)method to deposit uniform Pd nanoparticles((2.5±0.6)nm)on CeO2 nanorods(PdNPs/CeO2-ECD)through the interface redox reaction between the reduced CeO2 and Na2PdCl4.Pd NPs/CeO2-ECD exhibits a stronger electronic metal-support interaction(EMSI)evidenced by higher reducibility and stronger anti-sintering capability at high temperatures,compared to that prepared by the conventional impregnation method.Such an EMSI effect of PdNPs/CeO2-ECD significantly improves its catalytic activity in CO oxidation.Besides,the chlorine residue-free catalysts through ECD process avoid the deleterious effect of chlorine on CO oxidation.This ECD process can further be extended to deposit various uniform nanoscaled noble metals(Au,Ag,Pt,Ru,Rh,etc.)on CeO2,which may deliver their potentials in advanced catalysis.
基金the financial support from Joint Fund U1732267 of the National Natural Science Foundation of Chinathe Strategic Priority Research Program of Chinese Academy of Sciences(XDB17000000)+2 种基金the National Key R&D Program of China(2017YFB0602500)the National Natural Science Foundation of China(Grant no.21503218)DICP DMTO201306(Grant no.DICP DMTO201306)
文摘Cobalt carbide has recently been reported to catalyse the FTO con version of syngas with high selectivity for the production of lower olefins (C2-C4). Clarifying the formation process and atomic structure of cobalt carbide will help understand the catalytic mechanism of FTO. Herein, hydrogenati on of carb on monoxide was investigated for cobalt carbide synthesized from CoMn catalyst, followed by X-ray diffraction, transmission electron microscopy, temperature programmed reaction and in situ X-ray absorption spectroscopy. By monitoring the evolution of cobalt carbide during syngas conversion, the wavelet transform results give evidenee for the formation of the cobalt carbide and clearly demonstrate that the active site of catalysis was cobalt carbide.
基金supported from the National Natural Science Foundation of China,Grant/Award Number:U1732267,21503218.
文摘Cobalt carbide(Co2C)was considered as potential catalysts available for large-scale industrialization of transforming syngas(H2 and CO)to clean fuels.Herein,we successfully synthesized Co-based catalysts with MnO supported,to comprehend the effects of Co2C for Fischer–Tropsch synthesis(FTS)under ambient conditions.The huge variety of product selectivity which was contained by different active sites(Co and Co2C)has been found.Furthermore,density functional theory(DFT)shows that Co2C is efficacious of CO adsorption,whereas is weaker for H adsorption than Co.Combining the advantages of Co and Co2C,the catalyst herein can not only obtain more C5+products but also suppress methane selectivity.It can be a commendable guide for the design of industrial application products in FTS.
基金This work was financially supported by Shenzhen Nobel Prize Scientists Laboratory Project(No.C17213101)Guangdong Provincial Key Laboratory of Catalysis(No.2020B121201002)+6 种基金Guangdong Provincial Key Laboratory of Energy Materials for Electric Power(No.2018B030322001)China Postdoctoral Science Foundation(No.2018M642133,X.Y.Z.)Post-doctorate Scientific Research Fund for staying(coming to)Shenzhen(No.K21217502,X.Y.Z.)the National Natural Science Foundation of China(No.21671096,Z.G.L.)Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials(No.ZDSYS20200421111401738,Z.G.L.)The authors also acknowledge the assistance of Southern University of Science and Technology Core Research Facilities(SUSTech CRF)Key Laboratory of Energy Conversion and Storage Technologies(Southern University of Science and Technology).
文摘Herein,we prepared a bimetallic layered double hydroxide(FeCo LDH)featuring a dandelion-like structure.Anchoring of CeO_(2)onto FeCo LDH produced interfaces between the functionalizing CeO_(2)and the parent LDH.Comparative electrochemical studies were carried out.Onset potential,overpotential,and Tafel slope point to the superior oxygen-evolving performance of CeO_(2)-FeCo LDH with respect to FeCo LDH,therefore,demonstrating the merits of CeO_(2)functionalization.The electronic structures of Fe,Co,and Ce were analyzed by X-ray photoelectron spectroscopy(XPS)and electron energy loss spectroscopy(EELS)from which the increase of Co^(3+)and the concurrent lowering of Ce^(4+)were established.With the use of CeO_(2)-FeCo LDH,accelerated formation at a sizably reduced potential of Co-OOH,one of the key intermediates preceding the release of O_(2)was observed by in situ Raman spectroscopy.We now have the atomic-level and location-specific evidence,the increase of the active Co^(3+)across the interface to correlate the enhanced catalytic performance with CeO_(2)functionalization.
文摘The strategy of element substitution is an effective way to tune the electronic structures of the active sites in catalysts, thereby leading to improvements in both the catalytic activity and stability. Herein, we design and synthesize pyrite-type nickel/phosphorus co-doped CoS2 nanowires on carbon cloth （NiCoPS/CC） as efficient and durable electrodes for water electrolysis. Introduction of nickel and phosphorus produced stepwise and superb enhancement of the performance of the electrodes in the hydrogen evolution reaction due to regulation of the electronic structures of the active sites of the catalyst and accelerated charge transfer over a wide pH range （0-14）. The NiCoPS/CC electrodes also delivered a nearly undecayed catalytic current density of 10 mA.cm-2 at a low overpotential of 230 mV for oxygen evolution due to in situ formation of surficial Ni-Co oxo/hydroxide in 1.0 M KOH. Thus, the NiCoPS/CC electrodes gave rise to a catalytic current density of 10 mA·cm-2 for overall water splitting at potentials as low as 1.54 V during operation over 100 h in 1.0 M KOH with a Faradic efficiency of ~100%.
基金supported by the National Natural Science Foundation of China(21201138)the National Basic Research Program of China(2012CB619401)
文摘Silicon-based electrodes have attracted great attention in the artificial photosynthetic systems that mimic natural photosynthesis and directly convert the solar energy into chemical energy. Despite significant efforts to date,catalytic stability of the silicon photoelectrodes is limited by their poor electrochemical stability. The formation of passivation or protective layers provides a feasible strategy to improve the photocatalytic stability of silicon photoelectrodes. Many candidates including metals, metal oxides, metal silicides and polymers have been explored as the protection layers for silicon photoelectrodes. The present review gives a concise overview of the protected silicon photoanodes for water oxidation with a focus on the relationship between the structural architecture of silicon photoanodes and their photocatalytic activity and stability.
文摘To further investigate the influence of metal ions on the allylic rearrangement of 3,4,5,6-tetrahydrophthalic an- hydride during the hydrothermal reaction, metal ions such as manganese（Ⅱ）, zinc（Ⅱ） and cadmium（Ⅱ） have been employed in the synthesis, which leads to the formation of three new lamellar coordination polymers, [MnⅡs（μ3-OH）3（1-chec）（1,2-chedc）（2,3-chedc）2（H20）] （3Mn）, [ZnⅡs（μ3-OH）3（1-chec）（1,2-chedc）（2,3-chedc）2（H20）] （4Zn）, and [CdⅡ3（μ3-OH）2（1,2-chedc）2] （5Cd） （1-chec=cyclohexene-l-carboxylate, 1,2-chedc=cyclohexene-1,2- dicarboxylate, 2,3-chedc=cyclohexene-1,2-dicarboxylate）. Interestingly, the allylic rearrangement reaction is metal-dependent, which occurs only in 3Mn and 4Zn, resulting in the formation of one chiral carbon atom of the corresponding dicarboxylate ligands in both compounds. In addition, the magnetic property of compound 3Mn was studied, which revealed strong antiferromagnetic interactions between the metal centers.
