CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ziqiang Wang,Guanghui Yang,Pengjun Tian,Xinmiao Li,Kai Deng,Hongjie Yu,You Xu,Hongjing Wang,Liang Wang
The use of thermodynamically more favorable sulfion oxidation reaction (SOR) to replace sluggish oxygen evolution reaction is an effective method for energy-saving production of hydrogen. Herein, we propose the synthesis of organic–inorganic hybrid through the modification of 1-hydroxyethylidene-1,1-diphosphonic acid on Rh metallene (HEDP-Rh metallene) as a bifunctional electrocatalyst for hydrogen evolution reaction (HER) and SOR. The modification of hydrophilic HEDP can effectively promote the water adsorption, thereby accelerating the mass/electron transfer at the interface. The HEDP-Rh metallene requires low overpotentials of 30 mV at 10 mA cm −2 for HER and 0.538 V at 100 mA cm −2 for SOR. In HER-SOR coupled reaction, HEDP-Rh metallene drives the current density of 100 mA cm −2 at 1.08 V for concurrent production of hydrogen and sulfur, highlighting energy-efficient hydrogen production and sulfur recycle.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2023
·
IF 13.1
Qiqi Mao,Wenxin Wang,Kai Deng,Hongjie Yu,Ziqiang Wang,You Xu,Xiaonian Li,Liang Wang,Hongjing Wang
Utilizing the hydrazine-assisted water electrolysis for energy-efficient hydrogen production shows a promising application, which relies on the development and design of efficient bifunctional electrocatalysts . Herein, we reported a low-content Pt-doped Rh metallene (Pt-Rhene) for hydrazine-assisted water electrolysis towards energy-saving hydrogen (H 2 ) production, where the ultrathin metallene is constructed to provide enough favorable active sites for catalysis and improve atom utilization. Additionally, the synergistic effect between Rh and Pt can optimize the electronic structure of Rh for improving the intrinsic activity. Therefore, the required overpotential of Pt-Rhene is only 37 mV to reach a current density of −10 mA cm −2 in the hydrogen evolution reaction (HER), and the Pt-Rhene exhibits a required overpotential of only 11 mV to reach a current density of 10 mA cm −2 in the hydrazine oxidation reaction (HzOR). With the constructed HER-HzOR two-electrode system, the Pt-Rhene electrodes exhibit an extremely low voltage (0.06/0.19/0.28 V) to achieve current densities of 10/50/100 mA cm −2 for energy-saving H 2 production, which greatly reduces the electrolysis energy consumption. Moreover, DFT calculations further demonstrate that the introduction of Pt modulates the electronic structure of Rh and optimizes the d -band center, thus enhancing the adsorption and desorption of reactant/intermediates in the electrocatalytic reaction.
研究领域:
材料科学
·
电催化
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Kai Deng,Qiqi Mao,Wenxin Wang,Peng Wang,Ziqiang Wang,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Seawater splitting is considered as a promising way to replace water splitting for H 2 production due to the enrichment of seawater resources. However, the development of this technology has been greatly hampered by the lack of efficient electrocatalysts and the detrimental effects of chlorine electrochemistry. Herein, we report a defect-rich low-crystalline Rh metallene ( l -Rh metallene) with an amorphous/crystalline hetero-phase structure for seawater electrolysis, where chlorine generation is avoided by replacing the oxygen evolution reaction (OER) with the hydrazine oxidation reaction (HzOR). Benefiting from the large surface-to-volume ratio, abundant active sites and unique electronic structure, the l -Rh metallene exhibits out-standing catalytic activity for both hydrogen evolution reaction (HER, −38 mV at 10 mA cm −2 ) and HzOR (−2 mV at 10 mA cm −2 ). Notably, an ultra-low voltage of only 28 mV is required to achieve 10 mA cm −2 in two-electrode hydrazine-assisted seawater splitting system.
研究领域:
材料科学
·
电化学
·
可再生能源
✓ 已验证
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2022
·Vol. 32
·期 31
·2201081
·
IF 19.924
Qiqi Mao,Kai Deng,Hongjie Yu,You Xu,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Designing efficient and durable electrocatalysts for seawater electrolysis shows a great research prospect, but it remains a significant challenge. Herein, we report the partially hydroxylated Rh metallene (Rh/RhOOH metallene) with porous, ultrathin, defect-rich and hetero-phase structure for ethylene glycol (EG)-assisted seawater electrolysis. In parallel, the unique redox effect of RhOOH species and EG as well as the electroreduction effect riggers the in situ reconstruction for the catalyst during electrocatalysis, which further produces active Rh species to optimize the catalytic activity center and surface catalytic reaction. Benefiting from the unique metallene structure and the Rh/RhOOH heterogeneous structure, the Rh/RhOOH metallene exhibits superior electrocatalytic performance towards hydrogen evolution reaction (HER, overpotential of 29 mV) and EG oxidation reaction (EGOR, specific activity of 1.051 mA cm –2 ). Encouragingly, in the constructed EG-assisted seawater electrolysis system, the Rh/RhOOH metallene only needs a low cell voltage of 0.678 V to achieve a current density of 10 mA cm –2 for energy-saving H 2 production, which significantly reduces energy consumption compared to conventional seawater electrolysis.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Mao Qiqi,Mu Xu,Wang Wenxin,Deng Kai,Yu Hongjie,Wang Ziqiang,Xu You,Wang Liang,Wang Hongjing
Organic electrocatalytic conversion is an essential pathway for the green conversion of low-cost organic compounds to high-value chemicals, which urgently demands the development of efficient electrocatalysts. Here, we report a Cu single-atom dispersed Rh metallene arrays on Cu foam for cathodic nitrobenzene electroreduction reaction and anodic methanol oxidation reaction. In the coupled electrocatalytic system, the Cu single-atom -Rh metallene arrays on Cu foam requires only the low voltages of 1.18 V to reach current densities of 100 mA cm −2 for generating aniline and formate, with up to ~100% of nitrobenzene conversion/ aniline selectivity and over ~90% of formate Faraday efficiency, achieving synthesis of high-value chemicals. Density functional theory calculations reveal the electron effect between Cu single-atom and Rh host and catalytic reaction mechanism. The synergistic catalytic effect and H*-spillover effect can improve catalytic reaction process and reduce energy barrier for reaction process, thus enhancing electrocatalytic reaction activity and target product selectivity.
研究领域:
化学工程
·
电化学
·
催化
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）