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第八届新型太阳能材料科学与技术学术研讨会

作者： Yang Sun Xinli Wang Hao-Yi Wang Shuai Yuan Yi Wang Xi-Cheng Ai Jian-Ping Zhang Department of Chemistry Renmin University of China

The strategy of Lewis base modification has been shown to be rather effective in fabricating high-quality perovskite crystals, however, the underlying mechanisms remain controversial owing to the lack of any systematic characterization of the crystallization process. Herein, we report a novel non-invasive optical technique, referred to as the vertical reflection-type in-situ, real-time absorption spectroscopy, to investigate the mechanisms of Lewis base-mediated optimization of perovskite crystallinity by visualizing the entire energetic landscape of crystal growth. We show that by virtue of the urea additive, a prototypical Lewis base, the growth kinetics is accelerated prominently by reducing the activation energy from 73.7 kJ/mol to 41.7 kJ/mol. Besides, the self-passivation of structural disorders during thermal annealing is identified, which is shown to be further strengthened by urea modification towards a shallower distribution of trap states.

关键词： in-situ spectroscopy metal halide perovskite Lewis-base modification self-passivation crystallization kinetics

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Electrochemical transformation of biomass-derived oxygenates

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Science China Chemistry 2023年第4期66卷 1011-1031页

作者： Peng Zhou Jie Zhang School of Chemistry Monash UniversityClaytonVictoria 3800Australia

Replacing conventional fossil resources with renewable raw materials for chemical production and energy generation is crucial for achieving the carbon-neutral goal and alleviating the emerging energy *** has been considered as one of the most promising candidates for this purpose owing to its great natural abundance and inherent ability to fix CO_(2) in the form of multicarbon ***,biomass conversion through an electrochemical route is intriguing because of its operability near ambient conditions,flexible scalability(suitable for distributed manufacturing and even domestic use)and green generation of oxidative or reductive equivalents instead of wasteful and possibly explosive or flammable ***,recent progress in electrochemical transformation of biomass,including hydrogenation and amination,is reviewed with the emphasis on catalysts and strategies for enhancing catalytic *** advances in mechanistic understanding using in-situ spectroscopy are also briefly ***,recommendations for the directions for future development are also provided.

关键词： biomass utilization electrochemical hydrogenation reductive amination catalyst in-situ spectroscopy mechanism

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Selectively converting CO_(2) to HCOOH on Cu-alloys integrated in hematite-driven artificial photosynthetic cells

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Journal of Energy Chemistry 2023年第4期79卷 601-610页

作者： Jiwu Zhao Liang Huang Lan Xue Zhenjie Niu Zizhong Zhang Zhengxin Ding Rusheng Yuan Xu Lu Jinlin Long State Key Laboratory of Photocatalysis on Energy and Environment College of ChemistryFuzhou UniversityFuzhou 350116FujianChina Clean Combustion Research Center(CCRC) Division of Physical Sciences and EngineeringKing Abdullah University of Science and Technology(KAUST)Thuwal 23955-6900Saudi Arabia

The integration of electrochemical CO_(2)reduction(CO_(2)RR) and photoelectrochemical water oxidation offers a sustainable access to valuable chemicals and fuels. Here, we develop a rapidly annealed hematite photoanode with a photocurrent density of 2.83 mA cm^(-2)at 1.7 VRHEto drive the full-reaction. We also present Cu-alloys electrocatalysis extended from CuInSnS4, which are superior in both activity and selectivity for CO_(2)RR. Specifically, the screened CuInSn achieves a CO_(2)to HCOOH Faradaic efficiency of 93% at a cell voltage of-2.0 V by assembling into artificial photosynthesis cell. The stability test of IT exhibits less than 3% degradation over 24 h. Furthermore, in-situ Raman spectroscopy reveals that both CO_(3)^(-2)and CO_(2)are involved in CO_(2)RR as reactants. The preferential affinity of C for H in the ^(*)HCO_(2)intermediate enables an improved HCOOH-selectivity, highlighting the role of multifunctional Cu in reducing the cell voltage and enhancing the photocurrent density.

关键词： CO_(2)reduction Rapid annealing Fe_(2)O_(3)photoanode CuInSnS_(4) in-situ spectroscopy

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