沙特基础工业公司（SABIC）近日荣获2015年度责任关怀优异奖（Responsible Care Merit Award）,以表彰其在帮助关键利益相关方及所在社区实现可持续发展,并创造持续价值方面的卓越贡献.这是继2013年首次获奖后,SABIC在华第二度荣膺这一...沙特基础工业公司（SABIC）近日荣获2015年度责任关怀优异奖（Responsible Care Merit Award）,以表彰其在帮助关键利益相关方及所在社区实现可持续发展,并创造持续价值方面的卓越贡献.这是继2013年首次获奖后,SABIC在华第二度荣膺这一殊荣.展开更多
Triggering structural asymmetry can induce charge redistribution and modify electronic structures,which is of great significance for the design of high-performance hydrogen oxidation reaction(HOR)electrocatalysts.Here...Triggering structural asymmetry can induce charge redistribution and modify electronic structures,which is of great significance for the design of high-performance hydrogen oxidation reaction(HOR)electrocatalysts.Herein,we propose a dual anion-induced strategy to create an innovative RuS_(2)-RuO_(2)heterostructure featuring abundant S-Ru-O interfaces(RuS_(2)-RuO_(2)@C).This RuS_(2)-RuO_(2)@C demonstrates an impressive mass activity of 2.61 mAμg_(RU)^(-1)and an exchange current density of 2.96 mA cm^(-2),surpassing Pt/C and other comparative samples by over 20 times.Durability assessments confirm the superior stability of RuS_(2)-RuO_(2)@C,with only minimal performance loss during operation.Density functional theory(DFT)calculations indicate that the asymmetric S-Ru-O configuration optimizes the interfacial electronic structure and shifts the d-band center closer to the Fermi level,effectively reducing the energy barrier of the rate-determining step(RDS)in the alkaline HOR process.Moreover,in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)characteristics disclose the formation of a substantial hydrogen bond network at the S-Ru-o interface,which aids in the desorption of H_(2)O_(ad)and facilitates the vital Volmer step in the HOR pathway.展开更多
Amorphous bimetallic borides,as a new generation of catalytic nanomaterials with modifiable electronic properties,are of great importance in the design of high-efficiency catalysts for NaBH_(4) hydrolysis.This study s...Amorphous bimetallic borides,as a new generation of catalytic nanomaterials with modifiable electronic properties,are of great importance in the design of high-efficiency catalysts for NaBH_(4) hydrolysis.This study synthesizes an amorphous Co_(3)B-Mo_(2)B_(5) catalyst using a self-sacrificial template strategy and NaBH_(4) reduction for both NaBH_(4) hydrolysis and the reduction of 4-nitrophenol.The catalyst delivers an impressive hydrogen generation rate of 7690.5 mL min^(-1) g^(-1) at 25℃,coupled with a rapid reaction rate of 0.701 min^(-1) in the reduction of 4-nitrophenol.The enhanced catalytic performance is attributed to the unique amorphous structure and the electron rearrangement between Co_(3)B and Mo_(2)B_(5).Experimental and theoretical analyses suggest electron transfer from Co_(3)B to the Mo_(2)B_(5),with the electron-deficient Co_(3)B site favoring BH_(4)^(-) adsorption,while the electron-rich Mo_(2)B_(5) site favoring H_(2)O adsorption,Furthermore,Co_(3)B-Mo_(2)B_(5) demonstrated potential for energy applications,delivering a power output of 0.3 V in a hydrogen-air fuel cell.展开更多
Designing exceptional-performance and long-lasting oxygen reduction reaction(ORR)catalysts is a critical challenge for the development of rechargeable Zn-air batteries(ZABs).In this study,we introduce a metal-free ORR...Designing exceptional-performance and long-lasting oxygen reduction reaction(ORR)catalysts is a critical challenge for the development of rechargeable Zn-air batteries(ZABs).In this study,we introduce a metal-free ORR catalyst composed of F-N co-doped hollow carbon(FNC),specifically engineered to address the limitations of conventional catalysts.The FNC catalysts were synthesized using a template-assisted pyrolysis method,resulting in a hollow,porous architecture with a high specific surface area and numerous active sites.Concurrently,F doping optimized the electronic configuration of pyridinic nitrogen.The introduction of C-F bonds reduced the reaction energy barrier,and the resulting N-C-F configuration enhanced the stability of the nitrogen center.The catalyst exhibits outstanding ORR activity in alkaline media,exhibiting a half-wave potential(E_(1/2))of 0.87 V,surpassing that of commercial Pt/C(E_(1/2)=0.85 V).When applied to both aqueous and flexible ZAB configurations,the FNC catalyst achieved peak power densities of 172 and 85 mW cm^(-2),respectively,along with exceptional cycling stabilities exceeding 5300 and 302 h,respectively.This study establishes a novel approach for designing metal-free ORR catalysts and next-generation ZABs,particularly for use in flexible and wearable microelectronic devices.展开更多
Active and poisoning-resistant Ru-based electrocatalysts for the hydrogen oxidation reaction(HOR)are designed and fabricated by integrating Cu/Ru dual single atoms and alloy CuRu nanoparticles(N-(CuRu)_(NP+SA)@NC)thro...Active and poisoning-resistant Ru-based electrocatalysts for the hydrogen oxidation reaction(HOR)are designed and fabricated by integrating Cu/Ru dual single atoms and alloy CuRu nanoparticles(N-(CuRu)_(NP+SA)@NC)through a strategy involving weak chemical reduction and ammonia-assisted gas-phase nitridation.The resultant N-(CuRu)_(NP+SA)@NC electrocatalysts feature nitrogen atoms coordinated to both Cu and Ru metal atoms via strong N-metal interactions.Density functional theory calculations revealed that alloyed CuRu nanoparticles and monodispersed Cu atoms are vital for altering the electronic configuration of the host Ru elements.This finely tuned structure enhanced the adsorption of H and OH and promoted CO oxidation over the N-(CuRu)_(NP+SA)@NC electrocatalyst,resulting in high alkaline HOR activity,as evidenced by the higher exchange current density of 3.74 mA cm^(-2)and high mass activity of 3.28 mAμg_(Ru)^(-1),which are far superior to those of most Ru-based catalysts reported to date.Moreover,the N-(CuRu)_(NP+SA)@NC electrocatalysts are resistant to CO poisoning and can be used at a high concentration of 1000 ppm CO with no distinct decay in the activity,in stark contrast to the commercial Pt/C catalyst under the same conditions.展开更多
基金supported by the National Natural Science Foundation of China(no.52363028,21965005)the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001,2018GXNSFAA294077)the Guangxi Technology Base and Talent Subject(GUIKE AD23023004,GUIKE AD20297039).
文摘Triggering structural asymmetry can induce charge redistribution and modify electronic structures,which is of great significance for the design of high-performance hydrogen oxidation reaction(HOR)electrocatalysts.Herein,we propose a dual anion-induced strategy to create an innovative RuS_(2)-RuO_(2)heterostructure featuring abundant S-Ru-O interfaces(RuS_(2)-RuO_(2)@C).This RuS_(2)-RuO_(2)@C demonstrates an impressive mass activity of 2.61 mAμg_(RU)^(-1)and an exchange current density of 2.96 mA cm^(-2),surpassing Pt/C and other comparative samples by over 20 times.Durability assessments confirm the superior stability of RuS_(2)-RuO_(2)@C,with only minimal performance loss during operation.Density functional theory(DFT)calculations indicate that the asymmetric S-Ru-O configuration optimizes the interfacial electronic structure and shifts the d-band center closer to the Fermi level,effectively reducing the energy barrier of the rate-determining step(RDS)in the alkaline HOR process.Moreover,in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)characteristics disclose the formation of a substantial hydrogen bond network at the S-Ru-o interface,which aids in the desorption of H_(2)O_(ad)and facilitates the vital Volmer step in the HOR pathway.
基金supported by the National Natural Science Foundation of China(Nos.52363028,21965005)Natural Science Foundation of Guangxi(Nos.2021GXNSFAA076001,2018GXNSFAA294077)Guangxi Technology Base and Talent Subject(Nos.GUIKE AD23023004,GUIKE AD20297039)。
文摘Amorphous bimetallic borides,as a new generation of catalytic nanomaterials with modifiable electronic properties,are of great importance in the design of high-efficiency catalysts for NaBH_(4) hydrolysis.This study synthesizes an amorphous Co_(3)B-Mo_(2)B_(5) catalyst using a self-sacrificial template strategy and NaBH_(4) reduction for both NaBH_(4) hydrolysis and the reduction of 4-nitrophenol.The catalyst delivers an impressive hydrogen generation rate of 7690.5 mL min^(-1) g^(-1) at 25℃,coupled with a rapid reaction rate of 0.701 min^(-1) in the reduction of 4-nitrophenol.The enhanced catalytic performance is attributed to the unique amorphous structure and the electron rearrangement between Co_(3)B and Mo_(2)B_(5).Experimental and theoretical analyses suggest electron transfer from Co_(3)B to the Mo_(2)B_(5),with the electron-deficient Co_(3)B site favoring BH_(4)^(-) adsorption,while the electron-rich Mo_(2)B_(5) site favoring H_(2)O adsorption,Furthermore,Co_(3)B-Mo_(2)B_(5) demonstrated potential for energy applications,delivering a power output of 0.3 V in a hydrogen-air fuel cell.
文摘Designing exceptional-performance and long-lasting oxygen reduction reaction(ORR)catalysts is a critical challenge for the development of rechargeable Zn-air batteries(ZABs).In this study,we introduce a metal-free ORR catalyst composed of F-N co-doped hollow carbon(FNC),specifically engineered to address the limitations of conventional catalysts.The FNC catalysts were synthesized using a template-assisted pyrolysis method,resulting in a hollow,porous architecture with a high specific surface area and numerous active sites.Concurrently,F doping optimized the electronic configuration of pyridinic nitrogen.The introduction of C-F bonds reduced the reaction energy barrier,and the resulting N-C-F configuration enhanced the stability of the nitrogen center.The catalyst exhibits outstanding ORR activity in alkaline media,exhibiting a half-wave potential(E_(1/2))of 0.87 V,surpassing that of commercial Pt/C(E_(1/2)=0.85 V).When applied to both aqueous and flexible ZAB configurations,the FNC catalyst achieved peak power densities of 172 and 85 mW cm^(-2),respectively,along with exceptional cycling stabilities exceeding 5300 and 302 h,respectively.This study establishes a novel approach for designing metal-free ORR catalysts and next-generation ZABs,particularly for use in flexible and wearable microelectronic devices.
文摘Active and poisoning-resistant Ru-based electrocatalysts for the hydrogen oxidation reaction(HOR)are designed and fabricated by integrating Cu/Ru dual single atoms and alloy CuRu nanoparticles(N-(CuRu)_(NP+SA)@NC)through a strategy involving weak chemical reduction and ammonia-assisted gas-phase nitridation.The resultant N-(CuRu)_(NP+SA)@NC electrocatalysts feature nitrogen atoms coordinated to both Cu and Ru metal atoms via strong N-metal interactions.Density functional theory calculations revealed that alloyed CuRu nanoparticles and monodispersed Cu atoms are vital for altering the electronic configuration of the host Ru elements.This finely tuned structure enhanced the adsorption of H and OH and promoted CO oxidation over the N-(CuRu)_(NP+SA)@NC electrocatalyst,resulting in high alkaline HOR activity,as evidenced by the higher exchange current density of 3.74 mA cm^(-2)and high mass activity of 3.28 mAμg_(Ru)^(-1),which are far superior to those of most Ru-based catalysts reported to date.Moreover,the N-(CuRu)_(NP+SA)@NC electrocatalysts are resistant to CO poisoning and can be used at a high concentration of 1000 ppm CO with no distinct decay in the activity,in stark contrast to the commercial Pt/C catalyst under the same conditions.
