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A co-coordination strategy to realize janus-type bimetallic phosphide as highly efficient and durable bifunctional catalyst for water splitting

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Journal of Materials Science & Technology 2021年第15期74卷 11-20页

作者： Bin Wang Yuanfu Chen Qi Wu Yingjiong Lu Xiaojuan Zhang Xinqiang Wang Bo Yu DongXu Yang Wanli Zhang State Key Laboratory of Electronic Thin Films and Integrated Devices University of Electronic Science and Technology of ChinaChengdu 610054China School of Science and Institute of Oxygen SupplyTibet UniversityLhasa 850000China

In this work,a Janus-type dual-ligand metal-organic frameworks derived bimetallic(Fe,Co)P nanoparticles embedded carbon nanotube(CNT)skeleton(DLD-Fe Co P@CNT)is presented and synthesized via a facile"co-coordination synthesis"strategy.The DLD-Fe Co P@CNT hybrid shows much better performances for OER and HER with much lower Tafel slope of 39.6(57.1)m V dec-1,an overpotential of 286(166)m V@10 m A cm^(-2)and better stability for OER(HER)in 1 M KOH.Being both cathode and anode for water splitting,it requires only a low voltage of 1.67 V to obtain 10 mA cm^(-2)with nearly 100%faradaic efficiency,which is close to Pt/C//RuO_(2)cell.Density functional theory calculations based on the bimetallic phosphide(Fe_(0.3)Co_(0.7)P)model reveal that,compared with the monometallic Fe P or Co P,the enhanced catalytic activities of Fe_(0.3)Co_(0.7)P is mainly manifested in its free energy of H adsorption(GH*)closer to zero,larger binding strength for H2O and higher electrical conductivity.

关键词： bimetallic phosphide Bifunctional catalyst Overall water splitting DFT calculation

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DFT-assisted rational design of CoM_(x)P/CC(M=Fe,Mn,and Ni) as efficient electrocatalyst for wide pH range hydrogen evolution and oxygen evolution

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Nano Research 2022年第10期15卷 8897-8907页

作者： Xiangrui Zhang Chunyan Sun Shusheng Xu Mengru Huang Yi Wen Xue-Rong Shi School of Materials Engineering Shanghai University of Engineering ScienceShanghai 201620China

Rational design of highly active transition-metal phosphides for electrocatalyzing overall water splitting in a wide pH range assisted by first-principle calculations can efficiently save the developing cost and hence is quite attractive.Under the guidance of density-functional theory(DFT)calculations that the introduction of dopants(Fe,Mn,and Ni)into CoP could promote the hydrogen evolution reaction(HER)performances,a series of binder-free CoM_(x)P/carbon cloth(CC;M=Fe,Mn,and Ni;x=0,0.05,0.2,0.5,and 1)were fabricated.Both experimental measurements and DFT calculations confirm the electronic modulation of dopants.DFT calculations further reveal that the modulated electronic structure promotes the electronic conductivity,favors the adsorption of key species,and consequently promotes the electrochemical performances.As predicted,the bimetallic phosphides demonstrate excellent HER performances in alkaline,acidic,and alkaline simulated seawater solutions and also deliver excellent oxygen evolution reaction(OER)performances,overwhelming the commercial RuO_(2).Benefiting from the modulated electronic structure and the hierarchical structure with massive CoFe0.05P zero-dimensional(0D)quantum dots anchored on two-dimensional(2D)N-doped porous carbon,CoFe0.05P delivered the best HER in four kinds of electrolytes(ƞ10 of 73 mV in an alkaline simulated seawater solution)and OER in two kinds of electrolytes(ƞ10 of 264 mV in an alkaline solution)with excellent stability of 45 h in the alkaline solution.The assembled CoFe0.05P/CC//CoFe0.05P/CC with the electrodes folded by 180°can still maintain a low cell potential of 1.62 V at 10 mA·cm^(−2).This work proves the feasibility of the reported rational design strategy of developing efficient electrocatalysts for overall water splitting in a wide pH range.

关键词： bimetallic phosphide pH-universal hydrogen evolution reaction(HER) oxygen evolution reaction(OER) zero-dimensional(0D)/two-dimensional(2D) first-principle calculations

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Hierarchical NiMoP_(2)-Ni_(2)P with amorphous interface as superior bifunctional electrocatalysts for overall water splitting

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Journal of Materials Science & Technology 2021年第18期77卷 108-116页

作者： Gaoqi Tian Songrui Wei Zhangtao Guo Shiwei Wu Zhongli Chen Fuming Xu Yang Cao Zheng Liu Jieqiong Wang Lei Ding Jinchun Tu Hao Zeng State Key Laboratory of Marine Resource Utilization in South China Sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China College of Physics and Optoelectronic Engineering.Shenzhen University Shenzhen 518080China Qiongtai Normal University Haikou 571127China Department of Physics SUNY-BuffaloBuffaloNY14260USA

Producing highly efficient bifunctional catalyst for the generation of hydrogen and oxygen through overall water splitting is an emerging direction in electrocatalysis.Herein,a dandelion-like hierarchical NiMoP_(2)-Ni_(2)P(nanowire/nanoparticle)heterostructure was synthesized for efficient electrochemical water splitting.The NiMoP_(2)-Ni_(2)P heterostructures grown on carbon cloth as a freestanding integrated electrode exhibited excellent oxygen evolution reaction(OER)activity and hydrogen evolution reaction(HER)activities with low overpotentials(258 mV and 53 mV to reach 10 mA cm~(-2)for the OER and HER,respectively),and small Tafel slope(45 mV dec^(-1)and 58 mV dec^(-1)for the OER and HER,respectively).Moreover,the NiMoP_(2)-Ni_(2)P heterostructure can act as both anode and cathode catalysts for overall water splitting with low overall potential of 1.48 V at 10 mA cm~(-2).Density functional theory(DFT)combined with structural probes suggests that the amorphous heterogeneous interfaces play an essential role in enhanced catalytic performance.

关键词： bimetallic phosphide Amorphous interface Adsorption energy Hydrogen evolution reaction Oxygen evolution reaction Water splitting

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Effect of a second metal(Co,Fe, Mo and W) on performance of Ni_2P/SiO_2 for hydrodeoxygenation of methyl laurate

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Journal of Energy Chemistry 2016年第3期25卷 418-426页

作者： Zhengyi Pan Rijie Wang Ziyang Nie Jixiang Chen Tianjin Key Laboratory of Applied Catalysis Science and Technology Department of Catalysis Science and Engineering School of Chemical Engineering and Technology Tianjin University

NiP/SiOand bimetallic Ni MP/Si O2(M = Co, Fe, Mo, W; Ni/M atomic ratio=5) catalysts were prepared by the temperature-programmed reduction method. The catalysts and their precursors were characterized by means of UV–Vis DRS, H-TPR, XRD, TEM, CO chemisorption and NH-TPD. Their performance for the deoxygenation of methyl laurate was tested on a fixed-bed reactor. The results show that the main phase was NiP in all catalysts, and M(M = Co, Fe, Mo, W) entered the lattice of NiP forming solid solution. Different from Fe and Co, the introduction of Mo and W into NiP/SiOreduced the phosphide particle size and increased the acid amount. In the deoxygenation reaction, the turnover frequency of methyl laurate increased on the catalysts in the order of NiMoP/SiO, NiP/SiO, Ni WP/Si O2, NiFeP/SiOand NiCoP/SiO, which is influenced by the size of phosphide particles and the interaction between Ni and M(M = Fe, Co, Mo or W). The introduction of the second metal(especially Mo and W) into NiP/SiOpromoted the hydrodeoxygenation pathway. This is mainly attributed to the interaction between Ni and the second metal. Finally, the Ni MoP/SiOcatalyst was tested at 340 oC, 3 MPa, methyl laurate WHSV of 14 h-1and H/methyl laurate molar ratio of 25 for 132 h, and its deactivation took place. We found that the catalyst deactivation mainly resulted from carbonaceous deposit rather than the sintering of metal phosphide crystallites.

关键词： bimetallic phosphide Solid solution Methyl laurate Hydrodeoxygenation Decarbonylation

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