ACS Nano
·
2020
·
IF 14.588
Yuxuan Lin,Zhichao Huang,Xiaojie Wen,Wenhui Rong,Zhantao Peng,Mengxiao Diao,Lingbo Xing,Jingxin Dai,Xiong Zhou,Kai Wu
Among the multitudinous methodologies to steer on-surface reactions, less attention has been paid to the effect of externally introduced halogen atoms. Herein, highly selective trans-dehydrogenation coupling at the specific meta-C–H site of two poly(p-phenylene) molecules, p-quaterphenyl (Ph4) and p-quinquephenyl (Ph5), is achieved on Cu(111) by externally introduced bromine atoms. Scanning tunneling microscopy/spectroscopy experiments reveal that the formed molecular assembly structure at a stoichiometric ratio of 4:1 for Br to Ph4 or 5:1 for Br to Ph5 can efficiently promote the reactive collision probability to trigger the trans-coupling reaction at the meta-C–H site between two neighboring Ph4 or Ph5 molecules, leading to an increase in the coupling selectivity. Such Br atoms can also affect the electronic structure and adsorption stability of the reacting molecules. It is conceptually demonstrated that externally introduced halogen atoms, which can provide an adjustable halogen-to-precursor stoichiometry, can be employed to efficiently steer on-surface reactions.
研究领域:
表面化学
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纳米材料
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表面合成
·
物理化学
·
扫描探针显微学
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry C
·
2025
·
IF 5.1
Shuang Xu,Lei Yang,Congya Wang,Liwei Pan,Jing Zhang,Yaling Wang,Hexiang Zhong
With the rapid development of industry, large-scale fossil energy consumption leads to the increase of atmospheric CO2 concentration and the resultant deteriorating global warming. The electrochemical reduction of CO2 (ERCO2) technology is a potential strategy to achieve the CO2 emissions reduction and to realize carbon recycling. However, the lack of high product selective, active and stable catalysts is one of the remaining challenges for the industrial applications of ERCO2. Herein, an electrochemical oxidation-reduction reconstruction method is developed to reconstruct the copper network without extra Cu salt addition obtaining Cu2O-Cu (111) catalysts with nanoporous structures for improving the selectivity and activity of CH4 and C2H4 product. The oxidation-reduction reconstruction derived catalyst achieves improved faradaic efficiency of 56.63% for CH4 product and a partial current density of 41.6 mA cm-2 at -1.38 V (vs. RHE). The selectivity and activity toward C2H4 are also improved. The catalytic superiority originates from synergistic interplay between the Cu₂O-Cu heterogeneous interface and high electrochemical active surface area. Additionally, the presence of abundant oxygen vacancies at the Cu2O-Cu interface accelerate the electron transfer process and promote the high selectivity and activity toward CO2-to-CH4. This study paves a new way for enhancing the selectivity and activity of CO2 electrocatalytic conversion to CH4.
研究领域:
电化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Xia Bai,Jingmin Ge,Huanhuan Yang,Huiwen Tian,Xueqi Liu,Shiying Li,Zhikun Peng,Yaxi Li,Jiahao Wang,Hongpo Liu,Qun Xu
Building of grain boundary (GB) in Cu-based catalysts has been demonstrated to be an efficient strategy to control the product selectivity of electrochemical CO 2 reduction reaction (eCO 2 RR). However, the fabrication and modulation of GBs in Cu are still challenging. In this study, a series of bare Cu catalysts with controllable density of Cu(111) GBs were investigated systematically for eCO 2 RR. These catalysts exhibit superior eCO 2 RR performance for syngas production with a high FE of ∼80 % and tunable H 2 /CO ratio of 0.46–2.78. Three-dimensional wormlike Cu with abundant (111) GBs displays a stable H 2 /CO ratio of ∼0.5 over a wide potential range from −0.9 to −1.2 V ( vs. RHE). In situ Raman and ATR-SEIRAS spectroscopy combined with DFT calculations reveal that Cu(111) GBs enhance the adsorption of CO 2 , lower the energy barriers of CO 2 to *COOH and *CO, further highlighting the potential to control syngas production with desirable proportion over Cu-based catalysts.
研究领域:
材料科学
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电化学
·
催化
·
能源转化
✓ 已验证
DOI
高影响因子
Nature Nanotechnology
·
2020
·Vol. 15
·期 10
·848-853
·
IF 31.538
Jiang Lizhi,Liu Kunlong,Hung Sung-Fu,Zhou Lingyun,Qin Ruixuan,Zhang Qinghua,Liu Pengxin,Gu Lin,Chen Hao Ming,Fu Gang,Zheng Nanfeng
Hydrogen spillover is a well-known phenomenon in heterogeneous catalysis; it involves H 2 cleavage on an active metal followed by the migration of dissociated H species over an ‘inert’ support 1 , 2 , 3 , 4 , 5 . Although catalytic hydrogenation using the spilled H species, namely, spillover hydrogenation, has long been proposed, very limited knowledge has been obtained about what kind of support structure is required to achieve spillover hydrogenation 1 , 5 . By dispersing Pd atoms onto Cu nanomaterials with different exposed facets, Cu(111) and Cu(100), we demonstrate in this work that while the hydrogen spillover from Pd to Cu is facet independent, the spillover hydrogenation only occurs on Pd 1 /Cu(100), where the hydrogen atoms spilled from Pd are readily utilized for the semi-hydrogenation of alkynes. This work thus helps to create an effective method for fabricating cost-effective nanocatalysts with an extremely low Pd loading, at the level of 50 ppm, toward the semi-hydrogenation of a broad range of alkynes with extremely high activity and selectivity.
研究领域:
催化
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材料科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）