Achieving high activity and durability for the oxygen reduction reaction(ORR)with an ultra-low amount of platinum is significant to promote the widespread application of proton exchange membrane fuel cells(PEMFCs).Her...Achieving high activity and durability for the oxygen reduction reaction(ORR)with an ultra-low amount of platinum is significant to promote the widespread application of proton exchange membrane fuel cells(PEMFCs).Here we report a new ultrathin(∼1 nm)ternary PtNiGa alloy nanowires(PtNiGa NWs)electrocatalyst,in which the presence of gallium(Ga)enhances the oxidation resistance of platinum(Pt)and nickel(Ni)and suppresses the dissolution of Ni.The mass and specific activities of PtNiGa NWs are about 11.2 and 7.6 times higher than those of commercial Pt/C catalysts for ORR.Moreover,the mass activity of PtNiGa/C NWs nanocatalyst decreased only by 12.8%and largely retained its electrochemical surface area(ECSA)after 10,000 potential cycles,compared with 38%loss of ECSA for commercial Pt/C catalyst.Therefore,this work provides a general guideline for preparing ternary alloy electrocatalysts and enhancing the activity and stability of the cathode ORR reaction of PEMFCs.展开更多
Shaping crystalline porous materials such as metal organic frameworks （MOFs） and zeolites into two-dimensional （2D） nanosheet forms is highly desirable for developing high-performance molecular sieving membranes. ...Shaping crystalline porous materials such as metal organic frameworks （MOFs） and zeolites into two-dimensional （2D） nanosheet forms is highly desirable for developing high-performance molecular sieving membranes. However, conventional exfoliation-deposition is complex and challenging for the large-scale fabrication of nanosheet MOF tubular membranes. Here, for the first time, we report a direct growth technique by ZnO self-conversion and ammonia assistance to fabricate zeolitic imidazolate framework （ZIF） membranes consisting of 2D nanosheets on porous hollow fiber substrates; the membranes are suitable for large-scale industrial gas separation processes. The proposed fabrication process for ZIF nanosheet membranes is based on the localized self-conversion of a pre-deposited thin layer of ZnO in a ligand solution containing ammonium hydroxide as a modulator. The resulting ZIF 2D nanosheet tubular membrane is highly oriented and only 50 nm in thickness. It exhibits excellent molecular sieving performance, with high H2 permeance and selectivity for H2/CO2 separation. This technique shows great promise in MOF nanosheet membrane fabrication for large-scale molecular sieving applications.展开更多
基金supported by the National Youth Top-notch Talent Support Program of China,and the Sichuan Science and Technology Program(No.2020YJ0243)Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(No.2022-K28).
文摘Achieving high activity and durability for the oxygen reduction reaction(ORR)with an ultra-low amount of platinum is significant to promote the widespread application of proton exchange membrane fuel cells(PEMFCs).Here we report a new ultrathin(∼1 nm)ternary PtNiGa alloy nanowires(PtNiGa NWs)electrocatalyst,in which the presence of gallium(Ga)enhances the oxidation resistance of platinum(Pt)and nickel(Ni)and suppresses the dissolution of Ni.The mass and specific activities of PtNiGa NWs are about 11.2 and 7.6 times higher than those of commercial Pt/C catalysts for ORR.Moreover,the mass activity of PtNiGa/C NWs nanocatalyst decreased only by 12.8%and largely retained its electrochemical surface area(ECSA)after 10,000 potential cycles,compared with 38%loss of ECSA for commercial Pt/C catalyst.Therefore,this work provides a general guideline for preparing ternary alloy electrocatalysts and enhancing the activity and stability of the cathode ORR reaction of PEMFCs.
基金This work was supported by the National Natural Science Foundation of China （Nos. 21476039 and 21076030）. M. T. thanks the Marie S~odowska-Curie Individual Fellowship for a postdoctoral grant. A. J. H. and O. K. F. gratefully acknowledge funding from the U.S. Dept. of F.nerg~ Office of Science, Basic Energy Sciences Program （No. DE-FG02-08ER15967）. The authors also thank Professor Huanting Wang from Monash University for further revising the manuscript.
文摘Shaping crystalline porous materials such as metal organic frameworks （MOFs） and zeolites into two-dimensional （2D） nanosheet forms is highly desirable for developing high-performance molecular sieving membranes. However, conventional exfoliation-deposition is complex and challenging for the large-scale fabrication of nanosheet MOF tubular membranes. Here, for the first time, we report a direct growth technique by ZnO self-conversion and ammonia assistance to fabricate zeolitic imidazolate framework （ZIF） membranes consisting of 2D nanosheets on porous hollow fiber substrates; the membranes are suitable for large-scale industrial gas separation processes. The proposed fabrication process for ZIF nanosheet membranes is based on the localized self-conversion of a pre-deposited thin layer of ZnO in a ligand solution containing ammonium hydroxide as a modulator. The resulting ZIF 2D nanosheet tubular membrane is highly oriented and only 50 nm in thickness. It exhibits excellent molecular sieving performance, with high H2 permeance and selectivity for H2/CO2 separation. This technique shows great promise in MOF nanosheet membrane fabrication for large-scale molecular sieving applications.
