INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Yang Liu,Hailong Feng,Weiyi Li,Xueping Wang,Guoxiang Huang,Longxia Wang,Xingqiu Li,Yuxing Xie,Chenglu Liang
Catalysts in-situ reconstructed from transition metal sulfides for oxygen evolution reaction (OER) have been regarded as potential alternatives for the noble metal catalysts . Intriguingly, it was found that the self-optimized SO 4 2− @Cu doped Co(OH) 2 catalyst was reconstructed from bimetallic sulfide of CuCo 2 S 4 . During the OER process, the copper was partially leached and meantime doped into the in-situ generated Co(OH) 2 with SO 4 2− adsorption, while only oxides were discovered in counterparts of mono-metal sulfides. As a result, the SO 4 2− @Cu doped Co(OH) 2 catalyst exhibited superior OER performances, with low overpotentials of 211/272 mV to achieve the current densities of 10/100 mA cm −2 , exceeding the counterparts reconstructed from mono-metal sulfides. Experimental and theoretical results suggested that the in situ generated Cu doped Co(OH) 2 possessed thin and loosely layered structure with expanded lattice spacing (lattice spacing expanded from 0.28 nm to 0.46 nm) due to the SO 4 2− adsorption, making the intermediates more accessible to the active centers. In addition, the catalyst surface changed from hydrophobicity to super hydrophilicity , which greatly accelerated the mass transfer. This work indicated that the in-situ reconstruction process was greatly influenced by the interactions between metal sites and sulfide species, directly influencing the OER performances of the reconstructed catalysts.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Zi-Ye Liu,Jiu-Jiu Ge,Ji-Ming Hu
Nickel foam (NF) self-supported NiFe LDH electrodes have been widely studied for their excellent oxygen evolution reaction (OER) performance. However, the performance of electrodes synthesized via conventional electrodeposition or hydrothermal methods are still unsatisfactory owing to their insufficient specific surface area and suboptimal activity. In this study, we report NF-supported NiFe LDH electrodes directly derived from NF-supported-bimetallic MOF-74(NiFe). The as-prepared NiFe LDH exhibited a hierarchical structure and inherited the molecular level porosity of the MOF-74 precursor. The as-prepared electrode underwent self-optimization during the OER process, significantly increasing the electrochemical active surface area and providing numerous catalytic sites. In addition, the 2,5-dihydroxyterephthalate (DHTP) ligand released from MOF-74 during its dissociation chemically modified NiFe LDH. This ligand promoted the formation of Ni(III) and resisted Cl− corrosion. Thus, LDH-MOF74@NF outperformed almost all previously reported NiFe LDH@NF electrodes, exhibiting excellent OER performance and high durability in KOH and KOH/NaCl solutions with overpotentials of 244 mV and 254 mV at 100 mA cm−2, respectively.
研究领域:
材料科学
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电化学
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催化
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2024
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IF 5.4
Yanting Ma,Yan Tang,Yajuan Xu,Suisui Su,Shuzhen Chen,Shizheng Zheng,Changyuan Hu,Xin Li,Kejie Dai,Rongbin Zhang
Metal oxides are promising alkaline battery electrodes with high theoretical capacity, but the low energy density and poor stability make them far away from actual application. Herein, single Bi-MOF derived ultrastable Bi2O3@C and BiOCl@C anodes are architected via a two-for-one manner. Specifically, optimal Bi2O3@C anode with hierarchical and porous structure delivers high specific capacity (278.3 mAh g–1 at 1 A g–1) owing to the exposed electrochemical active sites, fast charge transfer, and efficient ion diffusion. More importantly, ultrahigh stability (110%, 5000 cycles) is achieved due to the in situ morphological self-optimization and oxygen vacancy creation. Similarly, BiOCl@C anode also displays remarkable capacity and ultralong cycling stability (94%, 15000 cycles) due to the conductive and protective carbon layer, abundant reactive centers, and ion transport channels. Moreover, the in situ phase transition of BiOCl to Bi2O2CO3 also contributes to the outstanding stability. Our work provides rational guidance for architecting high capacitive and ultrastable anodes for aqueous rechargeable alkaline battery.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Reaction Chemistry & Engineering
·
2021
·Vol. 7
·期 3
·590-598
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IF 4.239
Runzhe Liang,Xiaonan Duan,Jisong Zhang,Zhihong Yuan
In recent years, self-optimization strategies have been gradually utilized for the determination of optimal reaction conditions owing to their high convenience and independence from researchers' experience. However, most self-optimization algorithms still focus on homogeneous reactions or simple heterogeneous reactions. Investigations on complex heterogeneous gas–liquid–solid reactions are rare. Based on the Nelder–Mead simplex method and Bayesian optimization, this work proposes a reaction optimization framework for optimizing complex gas–liquid–solid reactions. Three gas–liquid–solid reactions including the hydrogenations of nitrobenzene, 3,4-dichloronitrobenzene, and 5-nitroisoquinoline are investigated, respectively. Reaction parameters (temperature, hydrogen pressure, liquid flow rate, and gas flow rate) are optimized. Compared with the traditional OVAT method, the proposed Bayesian based optimization algorithm exhibits remarkable performance with higher yields (0.998, 0.991 and 0.995, respectively) and computational efficiency.
研究领域:
化学工程
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人工智能应用
✓ 已验证
产品关联
DOI
高影响因子
Small Methods
·
2022
·Vol. 6
·期 8
·2200280
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IF 15.367
Binghao Zhang,Le Cheng,Libei Huang,Yu Tang,Yongjin Fang,Tao Li,Ruquan Ye,Qi Liu
Laser scribing technology is a straightforward technique to fabricate porous graphene, yet only conducted with polymeric precursors. Compared to polymers, molecular engineering of small organic molecules is much easier, which can be used to modify the graphene with tailored performance. Here we report the first employment of a laser to respectively transform small organic molecules, pentacene quinone and tetraazapentacene quinone (TAPQ), into graphene (P-LIG and N-LIG) as high-performance lithium-ion battery anodes. The TAPQ, as the N-fused molecular precursor, produces nitrogen-doped graphene. Both N-LIG and P-LIG exhibit significant self-enhancement of capacity upon cycling; the N-LIG anode delivers reversible capacities of 5863 mAh g -1 at 0.2 A g -1 and retains 1970 mAh g -1 at 2 A g -1 after another 500 cycles, which is the best performance for the graphene-type anode. Kinetics studies and structural characterizations verify that the surface- and diffusion-controlled processes are both progressively optimized, providing extra lithium storage upon cycling. It is also supported by small-angle X-ray scattering that the disordering level of micropores is increased upon cycling for N-LIG, corresponding to the enhancement of microporous level. Our work successfully develops a novel facile approach to fabricating heteroatom-doped microporous graphene exhibiting high performance and provides new insight into the lithium storage mechanism.
研究领域:
材料科学
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能源存储
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Energy & Environmental Science
·
2020
·Vol. 14
·期 2
·906-915
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IF 30.289
Dengfeng Cao,Daobin Liu,Shuangming Chen,Oyawale Adetunji Moses,Xingjia Chen,Wenjie Xu,Chuanqiang Wu,Lirong Zheng,Shengqi Chu,Hongliang Jiang,Changda Wang,Binghui Ge,Xiaojun Wu,Jing Zhang,Li Song
The ambiguous mechanism of electrocatalysts for the oxygen evolution reaction (OER) greatly hinders their industrial applications toward renewable and clean energy conversion. Here, we elaborately prepared a cobalt sulfide catalyst to perform a comprehensive study of the OER performance under neutral/alkaline conditions. The combination of synchrotron-based operando X-ray spectroscopic investigations and electron microscopy observations captured a chameleon-like structural self-optimization on the cobalt sulfide oxygen evolution electrocatalyst in both neutral and alkaline electrolytes. Driven by the actual working conditions (pH gradient, electrical potential, etc.), distinct catalytic sites could be activated dramatically. In particular, the CoOOH supported on a single-walled carbon nanotube (CoOOH-SWCNT) with residual S species was identified as the true catalyst under alkaline conditions rather than the entirely transformed CoOOH-SWCNT, while the oxygenated CoS-SWCNT (O-CoS-SWCNT) was formed as the true catalyst under neutral conditions. Undoubtedly, such a mechanism of opening different locks with different keys and its microstructural advantages together guarantee the high catalytic activity in different electrolytes. This work provides a promising catalyst as well as sheds light on the very essence of the structural self-optimization process of catalysts. It makes a significant contribution to the advancement of OER relevant studies in the future while providing new ideas for the fields of chemistry and catalysis.
研究领域:
电化学
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催化科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Science Bulletin
·
2025
·Vol. 70
·期 21
·3580-3588
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IF 21.1
Zhenyi Huang,Ruohan Yu,Jinshuai Liu,Yuxia Zhong,Lei Zhang,Liang Zhou
Silicon (Si), a promising high-capacity anode material for lithium-ion batteries, suffers from severe volume changes upon cycling, leading to rapid capacity fading. This study mitigates the capacity fading issue by introducing a surface SiN x layer on micron Si, which is in-situ converted into a Li x SiN y -based artificial solid electrolyte interphase (SEI). This artificial SEI not only effectively restricts SEI growth to the outmost surface, but also induces a self-optimized structural evolution of the inner Si from micron particles to nanoporous network within 20 cycles. This self-optimized nanoprous Si network exhibits low volume expansion and enhanced reaction kinetics. Consequently, the Si@SiN x /TiN demonstrates a high capacity, stable cycling, and good fast-charging capability.
研究领域:
材料科学
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电化学
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纳米科技
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能源存储
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电池技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2020
·Vol. 11
·期 1
·1-10
·
IF 12.121
Guan Daqin,Ryu Gihun,Hu Zhiwei,Zhou Jing,Dong Chung-Li,Huang Yu-Cheng,Zhang Kaifeng,Zhong Yijun,Komarek Alexander C.,Zhu Ming,Wu Xinhao,Pao Chih-Wen,Chang Chung-Kai,Lin Hong-Ji,Chen Chien-Te,Zhou Wei,Shao Zongping
Ion leaching from pure-phase oxygen-evolving electrocatalysts generally exists, leading to the collapse and loss of catalyst crystalline matrix. Here, different from previous design methodologies of pure-phase perovskites, we introduce soluble BaCl 2 and SrCl 2 into perovskites through a self-assembly process aimed at simultaneously tuning dual cation/anion leaching effects and optimizing ion match in perovskites to protect the crystalline matrix. As a proof-of-concept, self-assembled hybrid Ba 0.35 Sr 0.65 Co 0.8 Fe 0.2 O 3- δ (BSCF) nanocomposite (with BaCl 2 and SrCl 2 ) exhibits the low overpotential of 260 mV at 10 mA cm -2 in 0.1 M KOH. Multiple operando spectroscopic techniques reveal that the pre-leaching of soluble compounds lowers the difference of interfacial ion concentrations and thus endows the host phase in hybrid BSCF with abundant time and space to form stable edge/face-sharing surface structures. These self-optimized crystalline structures show stable lattice oxygen active sites and short reaction pathways between Co–Co/Fe metal active sites to trigger favorable adsorption of OH − species.
研究领域:
材料科学
·
电化学
·
催化
✓ 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）