The traditional automotive catalytic converter using commercial ceramic honeycomb carriers has many problems such as high back pressure,low engine efficiency,and high usage of precious metals.This study proposes a fou...The traditional automotive catalytic converter using commercial ceramic honeycomb carriers has many problems such as high back pressure,low engine efficiency,and high usage of precious metals.This study proposes a four-channel catalytic micro-reactor based on alumina hollow fiber membrane,which uses phase inversion method for structural molding and regulation.Due to the advantages of its carrier,it can achieve lower ignition temperature under low noble metal loading.With Pd/CeO_(2) at a loading rate of 2.3%(mass),the result showed that the reaction ignition temperature is even less than 160℃,which is more than 90℃ lower than the data of commercial ceramic substrates under similar catalyst loading and airspeed conditions.The technology in turn significantly reduces the energy consumption of the reaction.And stability tests were conducted under constant conditions for 1000 h,which proved that this catalytic converter has high catalytic efficiency and stability,providing prospects for the design of innovative catalytic converters in the future.展开更多
Proton exchange membrane fuel cells suffer from the sluggish kinetics of the oxygen reduction reaction(ORR)and the high cost of Pt catalysts.In the present work,a high‐performance ORR catalystbased on Fe,N,S‐doped p...Proton exchange membrane fuel cells suffer from the sluggish kinetics of the oxygen reduction reaction(ORR)and the high cost of Pt catalysts.In the present work,a high‐performance ORR catalystbased on Fe,N,S‐doped porous carbon(FeNS‐PC)was synthesized using melamine formaldehyderesin as C and N precursors,Fe(SCN)3as Fe and S precursors,and CaCl2as a template via a two‐stepheat treatment without a harsh template removal step.The results show that the catalyst treated at900℃(FeNS‐PC‐900)had a high surface area of775m2/g,a high mass activity of10.2A/g in anacidic medium,and excellent durability;the half‐wave potential decreased by only20mV after10000potential cycles.The FeNS‐PC‐900catalyst was used as the cathode in a proton exchangemembrane fuel cell and delivered a peak power density of0.49W/cm2.FeNS‐PC‐900therefore hasgood potential for use in practical applications.展开更多
In this study,a Mn-modified Pt-based catalyst loaded on nitrogen-doped Ketjen black(Mn-Pt/NKB)is prepared using a simple ethylene glycol reduction method.The size of Pt nanoparticles(NPs)is effectively controlled by d...In this study,a Mn-modified Pt-based catalyst loaded on nitrogen-doped Ketjen black(Mn-Pt/NKB)is prepared using a simple ethylene glycol reduction method.The size of Pt nanoparticles(NPs)is effectively controlled by doping with Mn and N.With the smallest average particle size of 1.7 nm,Mn-Pt/NKB demonstrates half-wave potentials of 0.890 and 0.688 V in the alkaline and neutral electrolytes,respectively,which are superior to those of commercial platinum on activated carbon(Pt/C).When applied as an air cathode in aluminum-air battery,it exhibits ultra-high power densities of 190(alkaline)and 26.2 mW·cm^(−2)(neutral).Moreover,the voltage remains stable after 5 h of discharge.The practical application performance of the Mn-Pt/NKB catalyst in an aluminum-air battery is better than that of commercial Pt/C.Furthermore,the oxygen reduction reaction(ORR)mechanism on surfaces with different particle sizes is analyzed using density functional theory.Oxygen cracking is the major pathway on the surface of the small particles with lower energy consumption of 0.5 eV,while water molecule cleavage is the major pathway on the surface of the large particles with higher energy consumption of 0.97 eV.The lower energy consumption of the oxygen cracking pathway further confirms the ORR mechanism for higher activity on small-sized surfaces.This study provides a direction for the rational design of Pt-based catalysts for ORR and sheds light on the commercial development of aluminum-air batteries.展开更多
To significantly reduce the cost of proton exchange membrane fuel cells, platinum-group metal (PGM)-free cathode catalysts are highly desirable. Current M-N-C (M: Fe, Co or Mn) catalysts are considered the most p...To significantly reduce the cost of proton exchange membrane fuel cells, platinum-group metal (PGM)-free cathode catalysts are highly desirable. Current M-N-C (M: Fe, Co or Mn) catalysts are considered the most promising due to their encouraging performance. The challenge thus has been their stability under acidic conditions, which has hindered their use for any practical applications. In this review, based on the author's research experience in the field for more than 10 years, current challenges and possible solutions to overcome these problems were discussed. The current Edisonian approach (i.e., trial and error) to developing PGM-free catalysts has been ineffective in achieving revolutionary breakthroughs. Novel synthesis techniques based on a more methodolo- gical approach will enable atomic control and allow us to achieve optimal electronic and geometric structures for active sites uniformly dispersed within the 3D architec- tures. Structural and chemical controlled precursors such as metal-organic frameworks are highly desirable for making catalysts with an increased density of active sites and strengthening local bonding structures among N, C and metals. Advanced electrochemical and physical characterization, such as electron microscopy and X-ray absorption spectroscopy should be combined with first principle density functional theory (DFT) calculations to fully elucidate the active site structures.展开更多
基金funded by the Natural Science Foundation of Jiangsu Province(BK20210252)。
文摘The traditional automotive catalytic converter using commercial ceramic honeycomb carriers has many problems such as high back pressure,low engine efficiency,and high usage of precious metals.This study proposes a four-channel catalytic micro-reactor based on alumina hollow fiber membrane,which uses phase inversion method for structural molding and regulation.Due to the advantages of its carrier,it can achieve lower ignition temperature under low noble metal loading.With Pd/CeO_(2) at a loading rate of 2.3%(mass),the result showed that the reaction ignition temperature is even less than 160℃,which is more than 90℃ lower than the data of commercial ceramic substrates under similar catalyst loading and airspeed conditions.The technology in turn significantly reduces the energy consumption of the reaction.And stability tests were conducted under constant conditions for 1000 h,which proved that this catalytic converter has high catalytic efficiency and stability,providing prospects for the design of innovative catalytic converters in the future.
基金supported by the National Basic Research Program of China (973 Program,2015CB932303)the National Natural Science Founda-tion of China (21373175,21621091)~~
文摘Proton exchange membrane fuel cells suffer from the sluggish kinetics of the oxygen reduction reaction(ORR)and the high cost of Pt catalysts.In the present work,a high‐performance ORR catalystbased on Fe,N,S‐doped porous carbon(FeNS‐PC)was synthesized using melamine formaldehyderesin as C and N precursors,Fe(SCN)3as Fe and S precursors,and CaCl2as a template via a two‐stepheat treatment without a harsh template removal step.The results show that the catalyst treated at900℃(FeNS‐PC‐900)had a high surface area of775m2/g,a high mass activity of10.2A/g in anacidic medium,and excellent durability;the half‐wave potential decreased by only20mV after10000potential cycles.The FeNS‐PC‐900catalyst was used as the cathode in a proton exchangemembrane fuel cell and delivered a peak power density of0.49W/cm2.FeNS‐PC‐900therefore hasgood potential for use in practical applications.
基金the National Natural Science Foundation of China(No.22078328)the Key Research Program of Nanjing IPE Institute of Green Manufacturing Industry。
文摘In this study,a Mn-modified Pt-based catalyst loaded on nitrogen-doped Ketjen black(Mn-Pt/NKB)is prepared using a simple ethylene glycol reduction method.The size of Pt nanoparticles(NPs)is effectively controlled by doping with Mn and N.With the smallest average particle size of 1.7 nm,Mn-Pt/NKB demonstrates half-wave potentials of 0.890 and 0.688 V in the alkaline and neutral electrolytes,respectively,which are superior to those of commercial platinum on activated carbon(Pt/C).When applied as an air cathode in aluminum-air battery,it exhibits ultra-high power densities of 190(alkaline)and 26.2 mW·cm^(−2)(neutral).Moreover,the voltage remains stable after 5 h of discharge.The practical application performance of the Mn-Pt/NKB catalyst in an aluminum-air battery is better than that of commercial Pt/C.Furthermore,the oxygen reduction reaction(ORR)mechanism on surfaces with different particle sizes is analyzed using density functional theory.Oxygen cracking is the major pathway on the surface of the small particles with lower energy consumption of 0.5 eV,while water molecule cleavage is the major pathway on the surface of the large particles with higher energy consumption of 0.97 eV.The lower energy consumption of the oxygen cracking pathway further confirms the ORR mechanism for higher activity on small-sized surfaces.This study provides a direction for the rational design of Pt-based catalysts for ORR and sheds light on the commercial development of aluminum-air batteries.
文摘To significantly reduce the cost of proton exchange membrane fuel cells, platinum-group metal (PGM)-free cathode catalysts are highly desirable. Current M-N-C (M: Fe, Co or Mn) catalysts are considered the most promising due to their encouraging performance. The challenge thus has been their stability under acidic conditions, which has hindered their use for any practical applications. In this review, based on the author's research experience in the field for more than 10 years, current challenges and possible solutions to overcome these problems were discussed. The current Edisonian approach (i.e., trial and error) to developing PGM-free catalysts has been ineffective in achieving revolutionary breakthroughs. Novel synthesis techniques based on a more methodolo- gical approach will enable atomic control and allow us to achieve optimal electronic and geometric structures for active sites uniformly dispersed within the 3D architec- tures. Structural and chemical controlled precursors such as metal-organic frameworks are highly desirable for making catalysts with an increased density of active sites and strengthening local bonding structures among N, C and metals. Advanced electrochemical and physical characterization, such as electron microscopy and X-ray absorption spectroscopy should be combined with first principle density functional theory (DFT) calculations to fully elucidate the active site structures.