One of the most primary challenges to achieve large-scale hydrogen generation from water electrolysis is the sluggish kinetics and noble metal dependence of cathodic hydrogen evolution reaction(HER).By considering the...One of the most primary challenges to achieve large-scale hydrogen generation from water electrolysis is the sluggish kinetics and noble metal dependence of cathodic hydrogen evolution reaction(HER).By considering the excellent water dissociation catalytic activity of Mo2C, abundant Pt/Mo2C interfaces were facilely engineered via galvanic replacement(gr) by using Mo/Mo2C nanosheets as self-sacrificed templates to alter the alkaline HER mechanism on Pt based catalyst. The rational designed interface-rich gr-Pt/Mo2C catalyst exhibited excellent activity with the overpotential to drive 10 mA/cm2 current density decreased by 18.5 mV compared with the commercial Pt/C catalyst. 34.3 mV/dec Tafel slope confirms the Volmer-Tafel HER route on gr-Pt/Mo2C in alkaline condition. Platinum utilization is calculated to be improved by 9.7 times by considered the low Pt loading in the gr-Pt/Mo2C catalyst. With its satisfied stability, the scalable gr-Pt/Mo2C catalyst shows promising application potential in industrial electrolysis systems.展开更多
The high cost of platinum(Pt)-group metal(PGM)-based catalysts used in proton-exchange membrane fuel cells(PEMFCs)poses a critical roadblock to their widespread adoption.Although using low PGM loading PEMFCs can large...The high cost of platinum(Pt)-group metal(PGM)-based catalysts used in proton-exchange membrane fuel cells(PEMFCs)poses a critical roadblock to their widespread adoption.Although using low PGM loading PEMFCs can largely address this challenge,high current density performance will be severely compromised consequently.To overcome this dilemma,we report the development of ultrathin platinum-cobalt nanowires(PtCoNWs)as the cathode catalysts for ultralow Pt loading and high-performance membrane electrode assembly(MEA).The Pt Co NWs delivered a record-high mass activity(MA)of 1.06±0.14 A mg_(Pt)^(-1) of Pt-alloy catalysts towards oxygen reduction reaction(ORR)in MEA,yielding an impressive total Pt utilization of 5.14 W_(rate)mg_(Pt)^(-1).The PtCoNWs retained a respectable endof-life MA of 0.45 Amg_(Pt)^(-1) after the 30,000 cycles square-wave accelerated stability test,which is still above the Department of Energy 2020 beginning-of-life target for catalysts.In-situ Xray absorption spectroscopy studies suggest that the high degree of alloying in the Pt Co NWs stabilizes the ultrathin structure and may contribute to the high ORR activity and power density performance in PEMFC.展开更多
A infrared light trapping structure combining front subwavelength gratings and rear ZnO：Al nanoparticles for a PtSi Schottky-barrier detector over a 3-5 μm waveband is theoretically investigated. By selecting the pr...A infrared light trapping structure combining front subwavelength gratings and rear ZnO：Al nanoparticles for a PtSi Schottky-barrier detector over a 3-5 μm waveband is theoretically investigated. By selecting the proper plasmonic material and optimizing the parameters for the proposed structure, the absorption of the PtSi layer is dramatically improved. The theoretical results show that this improvement eventually translates into an equivalent external quantum efficiency （EQE） enhancement of 2.46 times at 3-3.6 μm and 2.38 times at 3.6-5 μm compared to conventional structures. This improvement in the EQE mainly lies in the increase of light path lengths witifin the PtSi layer by the subwavelength grating diffraction and nanoparticle-scattering effects.展开更多
Catalyst utilization is an important determinant of proton exchange membrane fuel cell performance,and increasing the catalyst utilization is one of the most critical approaches to reducing the catalyst loading in PEM...Catalyst utilization is an important determinant of proton exchange membrane fuel cell performance,and increasing the catalyst utilization is one of the most critical approaches to reducing the catalyst loading in PEMFC.4-phase stochastic reconstruction method based on the variable-resolution Quartet Structure Generation Set(QSGS)algorithm is utilized to elucidate the influence of different parameters of electrode preparation,including the porosity,the dispersion degree of carbon agglomerate,ionomer content,and carbon support size,on the catalyst utilization in the catalyst layer.It was found that there exist optimal values for the porosity,dispersion degree of carbon agglomerate,ionomer content,and carbon support sizes in CLs and any deviations from these optimal values would lead to transport issues of electron,proton and mass within CLs.Taking electron,proton and mass transport into consideration simultaneously,the optimal Pt utilization is 46.55%among 48 cases in this investigation,taken at the carbon support diameter of 40 nm,the porosity of 0.4,the agglomerate spatial density of 25μm^(−3) and I/C at 0.7.The selection of porosity,ultrasonic dispersion technique and ionomer content for conventional electrode preparation requires compromises on mass,electron and proton transport,leading to catalyst utilization in CLs hardly exceeding 50%.Therefore,the next generation of catalyst layer design and preparation technology is desired.展开更多
基金financial support from the National Natural Science Foundation of China (Nos.21875224 and 21703211)the Natural Science Foundation of Zhejiang Province (No.LGG19B030001)。
文摘One of the most primary challenges to achieve large-scale hydrogen generation from water electrolysis is the sluggish kinetics and noble metal dependence of cathodic hydrogen evolution reaction(HER).By considering the excellent water dissociation catalytic activity of Mo2C, abundant Pt/Mo2C interfaces were facilely engineered via galvanic replacement(gr) by using Mo/Mo2C nanosheets as self-sacrificed templates to alter the alkaline HER mechanism on Pt based catalyst. The rational designed interface-rich gr-Pt/Mo2C catalyst exhibited excellent activity with the overpotential to drive 10 mA/cm2 current density decreased by 18.5 mV compared with the commercial Pt/C catalyst. 34.3 mV/dec Tafel slope confirms the Volmer-Tafel HER route on gr-Pt/Mo2C in alkaline condition. Platinum utilization is calculated to be improved by 9.7 times by considered the low Pt loading in the gr-Pt/Mo2C catalyst. With its satisfied stability, the scalable gr-Pt/Mo2C catalyst shows promising application potential in industrial electrolysis systems.
基金support from the Office of Naval Research(N000141812155)support from the National Science Foundation(DMREF 1437263)supported in part by the National Science Foundation through the UC Irvine Materials Research Science and Engineering Center(DMR-2011967)。
文摘The high cost of platinum(Pt)-group metal(PGM)-based catalysts used in proton-exchange membrane fuel cells(PEMFCs)poses a critical roadblock to their widespread adoption.Although using low PGM loading PEMFCs can largely address this challenge,high current density performance will be severely compromised consequently.To overcome this dilemma,we report the development of ultrathin platinum-cobalt nanowires(PtCoNWs)as the cathode catalysts for ultralow Pt loading and high-performance membrane electrode assembly(MEA).The Pt Co NWs delivered a record-high mass activity(MA)of 1.06±0.14 A mg_(Pt)^(-1) of Pt-alloy catalysts towards oxygen reduction reaction(ORR)in MEA,yielding an impressive total Pt utilization of 5.14 W_(rate)mg_(Pt)^(-1).The PtCoNWs retained a respectable endof-life MA of 0.45 Amg_(Pt)^(-1) after the 30,000 cycles square-wave accelerated stability test,which is still above the Department of Energy 2020 beginning-of-life target for catalysts.In-situ Xray absorption spectroscopy studies suggest that the high degree of alloying in the Pt Co NWs stabilizes the ultrathin structure and may contribute to the high ORR activity and power density performance in PEMFC.
基金supported by the National Natural Science Foundation of China(No.61471044)the Advanced Research Foundation of China(No.9140A02010114BQ01)
文摘A infrared light trapping structure combining front subwavelength gratings and rear ZnO：Al nanoparticles for a PtSi Schottky-barrier detector over a 3-5 μm waveband is theoretically investigated. By selecting the proper plasmonic material and optimizing the parameters for the proposed structure, the absorption of the PtSi layer is dramatically improved. The theoretical results show that this improvement eventually translates into an equivalent external quantum efficiency （EQE） enhancement of 2.46 times at 3-3.6 μm and 2.38 times at 3.6-5 μm compared to conventional structures. This improvement in the EQE mainly lies in the increase of light path lengths witifin the PtSi layer by the subwavelength grating diffraction and nanoparticle-scattering effects.
基金the funding support from the National Natural Science Foundation of China (22325903,22221003,and 22071225)the National Key Research and Development Program of China (2018YFA0702001)+1 种基金the Plan for Anhui Major Provincial Science&Technology Project (202203a0520013 and 2021d05050006)the USTC Research Funds of the Double First-Class Initiative (YD2060002032)。
基金This work is supported by National Key R&D Program of China(No.2021YFB4001303)the National Natural Science Foundation of China(No.52276206)+1 种基金the Science and Technology Commission of Shanghai Municipality(21DZ1208600)the Oceanic Interdisciplinary Program of Shanghai Jiao Tong University(SL2021ZD105).
文摘Catalyst utilization is an important determinant of proton exchange membrane fuel cell performance,and increasing the catalyst utilization is one of the most critical approaches to reducing the catalyst loading in PEMFC.4-phase stochastic reconstruction method based on the variable-resolution Quartet Structure Generation Set(QSGS)algorithm is utilized to elucidate the influence of different parameters of electrode preparation,including the porosity,the dispersion degree of carbon agglomerate,ionomer content,and carbon support size,on the catalyst utilization in the catalyst layer.It was found that there exist optimal values for the porosity,dispersion degree of carbon agglomerate,ionomer content,and carbon support sizes in CLs and any deviations from these optimal values would lead to transport issues of electron,proton and mass within CLs.Taking electron,proton and mass transport into consideration simultaneously,the optimal Pt utilization is 46.55%among 48 cases in this investigation,taken at the carbon support diameter of 40 nm,the porosity of 0.4,the agglomerate spatial density of 25μm^(−3) and I/C at 0.7.The selection of porosity,ultrasonic dispersion technique and ionomer content for conventional electrode preparation requires compromises on mass,electron and proton transport,leading to catalyst utilization in CLs hardly exceeding 50%.Therefore,the next generation of catalyst layer design and preparation technology is desired.
