Using photoelectrocatalytic CO_(2) reduction reaction(CO_(2)RR)to produce valuable fuels is a fascinating way to alleviate environmental issues and energy crises.Bismuth-based(Bi-based)catalysts have attracted widespr...Using photoelectrocatalytic CO_(2) reduction reaction(CO_(2)RR)to produce valuable fuels is a fascinating way to alleviate environmental issues and energy crises.Bismuth-based(Bi-based)catalysts have attracted widespread attention for CO_(2)RR due to their high catalytic activity,selectivity,excellent stability,and low cost.However,they still need to be further improved to meet the needs of industrial applications.This review article comprehensively summarizes the recent advances in regulation strategies of Bi-based catalysts and can be divided into six categories:(1)defect engineering,(2)atomic doping engineering,(3)organic framework engineering,(4)inorganic heterojunction engineering,(5)crystal face engineering,and(6)alloying and polarization engineering.Meanwhile,the corresponding catalytic mechanisms of each regulation strategy will also be discussed in detail,aiming to enable researchers to understand the structure-property relationship of the improved Bibased catalysts fundamentally.Finally,the challenges and future opportunities of the Bi-based catalysts in the photoelectrocatalytic CO_(2)RR application field will also be featured from the perspectives of the(1)combination or synergy of multiple regulatory strategies,(2)revealing formation mechanism and realizing controllable synthesis,and(3)in situ multiscale investigation of activation pathways and uncovering the catalytic mechanisms.On the one hand,through the comparative analysis and mechanism explanation of the six major regulatory strategies,a multidimensional knowledge framework of the structure-activity relationship of Bi-based catalysts can be constructed for researchers,which not only deepens the atomic-level understanding of catalytic active sites,charge transport paths,and the adsorption behavior of intermediate products,but also provides theoretical guiding principles for the controllable design of new catalysts;on the other hand,the promising collaborative regulation strategies,controllable synthetic paths,and the in situ multiscale characterization techniques presented in this work provides a paradigm reference for shortening the research and development cycle of high-performance catalysts,conducive to facilitating the transition of photoelectrocatalytic CO_(2)RR technology from the laboratory routes to industrial application.展开更多
The enhancement of activity and stability of noble metal-based catalysts for purification of auto-exhaust carbon particle(soot)oxidation remains a grand challenge under harsh reaction conditions.Herein,the encapsulate...The enhancement of activity and stability of noble metal-based catalysts for purification of auto-exhaust carbon particle(soot)oxidation remains a grand challenge under harsh reaction conditions.Herein,the encapsulated catalysts of platinum nanoparticles(NPs)confined in silicalite-1(S-1)zeolite were prepared by the ligand-protected in-situ synthesis method.The Pt NPs(4 nm)are located within the intersectional channels between the straight and the sinusoidal 10-ring channels of rigid S-1 zeolite and well stabilize inside the S-1 via Pt-O-Si bonds.The Pt@S-1 catalyst(0.38 wt.%of Pt loading)exhibits excellent performance(T_(50)=368℃,T_(50)corresponds to the temperatures at which 50%of soot conversion occurs)compared with the conventional Pt/S-1 catalyst during soot oxidation.The Pt@S-1 catalyst displays high long-term catalytic stability after the hydrothermal aging at 800℃for 10 h,and the deactivation rate of the Pt@S-1 catalyst is one-tenth that of the Pt/S-1 catalyst.In-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)calculations corroborated that the encapsulated Pt NPs in Pt@S-1 catalyst display a higher d-band center than the isolated Pt NPs,which enhances bonding strength for co-adsorption of NO and O_(2)molecules.The steric hindrance effect promotes the desorption of the critical intermediate of NO_(2),which is the key step to the NO_(2)-assistant catalytic mechanism for soot oxidation.The ligand-protected in-situ confinement synthesis of metal nanoparticle catalysts not only ensures high activity and stability but also paves the way for the development of effective catalysts for soot oxidation in practical applications.展开更多
基金supports from the National Natural Science Foundation of China(Grant Nos.12305372 and 22376217)the National Key Research&Development Program of China(Grant Nos.2022YFA1603802 and 2022YFB3504100)+1 种基金the projects of the key laboratory of advanced energy materials chemistry,ministry of education(Nankai University)key laboratory of Jiangxi Province for persistent pollutants prevention control and resource reuse(2023SSY02061)are gratefully acknowledged.
文摘Using photoelectrocatalytic CO_(2) reduction reaction(CO_(2)RR)to produce valuable fuels is a fascinating way to alleviate environmental issues and energy crises.Bismuth-based(Bi-based)catalysts have attracted widespread attention for CO_(2)RR due to their high catalytic activity,selectivity,excellent stability,and low cost.However,they still need to be further improved to meet the needs of industrial applications.This review article comprehensively summarizes the recent advances in regulation strategies of Bi-based catalysts and can be divided into six categories:(1)defect engineering,(2)atomic doping engineering,(3)organic framework engineering,(4)inorganic heterojunction engineering,(5)crystal face engineering,and(6)alloying and polarization engineering.Meanwhile,the corresponding catalytic mechanisms of each regulation strategy will also be discussed in detail,aiming to enable researchers to understand the structure-property relationship of the improved Bibased catalysts fundamentally.Finally,the challenges and future opportunities of the Bi-based catalysts in the photoelectrocatalytic CO_(2)RR application field will also be featured from the perspectives of the(1)combination or synergy of multiple regulatory strategies,(2)revealing formation mechanism and realizing controllable synthesis,and(3)in situ multiscale investigation of activation pathways and uncovering the catalytic mechanisms.On the one hand,through the comparative analysis and mechanism explanation of the six major regulatory strategies,a multidimensional knowledge framework of the structure-activity relationship of Bi-based catalysts can be constructed for researchers,which not only deepens the atomic-level understanding of catalytic active sites,charge transport paths,and the adsorption behavior of intermediate products,but also provides theoretical guiding principles for the controllable design of new catalysts;on the other hand,the promising collaborative regulation strategies,controllable synthetic paths,and the in situ multiscale characterization techniques presented in this work provides a paradigm reference for shortening the research and development cycle of high-performance catalysts,conducive to facilitating the transition of photoelectrocatalytic CO_(2)RR technology from the laboratory routes to industrial application.
基金support from the National Key Research and Development Program of China(No.2022YFB3504100)the National Natural Science Foundation of China(Nos.22376217,22208373,22272106,and 12305372)Key Laboratory of Jiangxi Province for Persistent Pollutants Prevention Control and Resource Reuse(No.2023SSY02061).
文摘The enhancement of activity and stability of noble metal-based catalysts for purification of auto-exhaust carbon particle(soot)oxidation remains a grand challenge under harsh reaction conditions.Herein,the encapsulated catalysts of platinum nanoparticles(NPs)confined in silicalite-1(S-1)zeolite were prepared by the ligand-protected in-situ synthesis method.The Pt NPs(4 nm)are located within the intersectional channels between the straight and the sinusoidal 10-ring channels of rigid S-1 zeolite and well stabilize inside the S-1 via Pt-O-Si bonds.The Pt@S-1 catalyst(0.38 wt.%of Pt loading)exhibits excellent performance(T_(50)=368℃,T_(50)corresponds to the temperatures at which 50%of soot conversion occurs)compared with the conventional Pt/S-1 catalyst during soot oxidation.The Pt@S-1 catalyst displays high long-term catalytic stability after the hydrothermal aging at 800℃for 10 h,and the deactivation rate of the Pt@S-1 catalyst is one-tenth that of the Pt/S-1 catalyst.In-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)calculations corroborated that the encapsulated Pt NPs in Pt@S-1 catalyst display a higher d-band center than the isolated Pt NPs,which enhances bonding strength for co-adsorption of NO and O_(2)molecules.The steric hindrance effect promotes the desorption of the critical intermediate of NO_(2),which is the key step to the NO_(2)-assistant catalytic mechanism for soot oxidation.The ligand-protected in-situ confinement synthesis of metal nanoparticle catalysts not only ensures high activity and stability but also paves the way for the development of effective catalysts for soot oxidation in practical applications.
