Recent advances in understanding mechanisms for the electrochemical reduction of carbon dioxide

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Recent progress in advanced core-shell metal-based catalysts for electrochemical carbon dioxide reduction

Electrochemical carbon dioxide reduction（CO₂RR） plays an important role in solving the problem of high concentration of CO₂in the atmosphere and realizing carbon cycle. Core-shell structure has many unique features including tandem catalysis, lattice strain effect, defect engineering, which exhibit great potential in electrocatalysis. In this review, we focus on the advanced core-shell metal-based catalysts（CMCs） for electrochemical CO₂RR. The recent progress of ...     

Recent advances of MXene as promising catalysts for electrochemical nitrogen reduction reaction

Electrochemical reduction of N_2,as an eco-friendly alternative,not only allows the use of protons in water as a source of hydrogen under mild conditions but also can be driven by renewable electric energy.The major challenge is to identify high-efficiency electrocatalysts.MXene is a new class of 2D transition metal carbides,nitrides,and carbonitrides that have received significant attention in electrocatalysis.The investigations on MXene in electrocatalytic nitrogen fixation are rapidly proceeding,and some breakthroughs have emerged ve ry recently due to MXenes' satisfacto ry catalytic activity.Here,the recent progress concerning the MXene-based catalysts for electrochemical N_2 reduction reaction(NRR) is highlighted.In regards to giving guidelines for exploring more efficient MXene-based catalysts for the NRR,the fabrication and surface modification of MXene are discussed.Besides,the shortcomings and challenges of current research are summarized and the future research directions are prospected.     

Modulation effect in adjacent dual metal single atom catalysts for electrochemical nitrogen reduction reaction

Nitrogen reduction reaction（NRR） is a clean mode of energy conversion and the development of highly efficient NRR electrocatalysts under ambient conditions for industrial application is still a big challenge.Metal-nitrogen-carbon（M-N-C） has emerged as a class of single atom catalyst due to the unique geometric structure, high catalytic activity, and clear selectivity. Herein, we designed a series of dual metal single atom catalysts containing adjacent M-N-C dual active centers（MN₄/M’N...     

Transition metal-nitrogen sites for electrochemical carbon dioxide reduction reaction

Electrochemical CO₂ reduction reaction (CO₂RR) powered by renewable electricity has emerged as the most promising technique for CO₂ conversion, making it possible to realize a carbon-neutral cycle. Highly efficient, robust, and cost-effective catalysts are highly demanded for the near-future practical applications of CO₂RR. Previous studies on atomically dispersed metal-nitrogen (M-N_x) sites constituted of earth abundant elements with maximum atom-utilization efficiency have demonstrated their performance towards CO₂RR. This review summarizes recent advances on a variety of M-N_x sites-containing transition metal-centered macrocyclic complexes, metal organic frameworks, and M-N_x-doped carbon materials for efficient CO₂RR, including both experimental and theoretical studies. The roles of metal centers, coordinated ligands, and conductive supports on the intrinsic activity and selectivity, together with the importance of reaction conditions for improved performance are discussed. The mechanisms of CO₂RR over these M-N_x-containing materials are presented to provide useful guidance for the rational design of efficient catalysts towards CO₂RR.     

Recent advances in carbon-based materials for electrochemical CO2 reduction reaction

The increase of atmospheric CO₂ concentration has caused many environmental issues. Electrochemical CO₂ reduction reaction（CO₂RR） has been considered as a promising strategy to mitigate these challenges. The electrocatalysts with a low overpotential, high Faradaic efficiency, and excellent selectivity are of great significance for the CO₂RR. Carbon-based materials including metal-free carbon catalysts and metal-based carbon catalysts have shown great p...     

Amino-metalloporphyrin polymers derived Fe single atom catalysts for highly efficient oxygen reduction reaction

Recently, nitrogen-doped porous carbon supported single atom catalysts(SACs) have become one of the most promising alternatives to precious metal catalysts in oxygen reduction reaction(ORR) due to their outstanding performance, especially those derived from porphyrin-based materials. However, most of them involve other metal residuals, which would cause the tedious pre-and/or post-treatment, even mislead the mechanistic investigations and active-site identification. Herein, we report a precursor-dilution strategy to synthesize Fe SACs through the Schiff-based reaction via co-polycondensation of amino-metalloporphyrin, followed by pyrolysis at high temperature. Systematic characterization results provide the compelling evidence of the dominant presence of atomically dispersed Fe-Nxspecies. Our catalyst shows superior ORR performance with positive half-wave potential(E_(1/2)=0.85 V vs. RHE) in alkaline condition and moderate activity(E_(1/2)=0.68 V vs. RHE) under the acidic condition, excellent methanol tolerance and good long-term stability. All the results indicate Fe SACs would be a promising candidate for replacing the precious Pt in metal-air batteries and fuel cells.     

Recent advances in catalytic conversion of carbon dioxide to propiolic acids over coinage-metal-based catalysts

The conversion of inexpensive,available C1 feedstock of carbon dioxide (CO2) into value-added fine chemicals via homogeneous or heterogeneous catalysis has attr...     

Nitrogen doped tin oxide nanostructured catalysts for selective electrochemical reduction of carbon dioxide to formate

Tin/tin oxide materials are key electrocatalysts for selective conversion of CO_2 to formate/formic acid.Herein we report a tin oxide material with nitrogen doping by using ammonia treatment at elevated temperature. The N doped material demonstrated enhanced electrocatalytic CO_2 reduction activity, showing high Faradaic efficiency(90%) for formate at -0.65 V vs. RHE with partial current density of 4 mA/cm~2.The catalysis was contributed to increased electron negativity of N atom compared to O atom. Additionally, the N-doped catalyst demonstrates sulfur tolerance with retained formate selectivity. The analysis after electrolysis shows that the catalyst structure partially converts to metallic Sn, and thus the combined Sn/N-SnO_2 is the key for the active CO_2 catalysis.     

Recent advances in carbon-based electrocatalysts for oxygen reduction reaction

Fuel cells are one of the most promising clean energy devices to substitute for fossil fuel in the future to alleviate energy crisis and environmental pollution.As the key reaction on the cathode in the fuel cells,oxygen reduction reaction(ORR) still requires efficient noble metal catalysts such as the comme rcial Pt/C to boost the reaction for its sluggish kinetics.Therefore,it is critical to design earth-abundant carbonbased catalysts with high efficiency and long-term stability to replace the...     

Recent advances in catalytic hydrogenation of carbon dioxide

Owing to the increasing emissions of carbon dioxide (CO(2)), human life and the ecological environment have been affected by global warming and climate changes. To mitigate the concentration of CO(2) in the atmosphere various strategies have been implemented such as separation, storage, and utilization of CO(2). Although it has been explored for many years, hydrogenation reaction, an important representative among chemical conversions of CO(2), offers challenging opportunities for sustainable development in energy and the environment. Indeed, the hydrogenation of CO(2) not only reduces the increasing CO(2) buildup but also produces fuels and chemicals. In this critical review we discuss recent developments in this area, with emphases on catalytic reactivity, reactor innovation, and reaction mechanism. We also provide an overview regarding the challenges and opportunities for future research in the field (319 references).     

Recent advances in carbon nanostructures prepared from carbon dioxide for high-performance supercapacitors

The burgeoning global economy during the past decades gives rise to the continuous increase in fossil fuels consumption and rapid growth of CO₂ emission,which demands an urgent exploration into green and sustainable devices for energy storage and power management.Supercapacitors based on activated carbon electrodes are promising systems for highly efficient energy harvesting and power supply,but their promotion is hindered by the moderate energy density compared with batteries.Therefore,scalable conversion of CO₂ into novel carbon nanostructures offers a powerful alternative to tackle both issues:mitigating the greenhouse effect caused by redundant atmospheric CO₂ and providing carbon materials with enhanced electrochemical performances.In this tutorial review,the techniques,opportunities and barriers in the design and fabrication of advanced carbon materials using CO₂ as feedstock as well as their impact on the energy-storage performances of supercapacitors are critically examined.In particular,the chemical aspects of various Cv2 conversion reactions are highlighted to establish a detailed understanding for the science and technology involved in the microstructural evolution,surface engineering and porosity control of CO₂-converted carbon nanostructures.Finally,the prospects and challenges associated with the industrialization of CO₂ conversion and their practical application in supercapacitors are also discussed.     

Molecular approaches to the electrochemical reduction of carbon dioxide

This article reviews recent progress in the exploitation of carbon dioxide as a chemical feedstock. In particular, the design and development of molecular complexes that can act as catalysts for the electrochemical reduction of CO(2) is highlighted, and compared to other biological, metal- and non-metal-based systems.     

Accelerating net-zero carbon emissions by electrochemical reduction of carbon dioxide

Electroreduction of CO₂ shows great potential for global CO₂ utilization and uptake when collaborated with renewable electricity. Recent advances have been achieved in fundamental understanding and electrocatalyst development for CO₂ electroreduction. We think this research area has progressed to the stage where significant efforts can focus on translating the obtained knowledge to the development of largescale electrolyzers, which have the potential to accelerat...     

Current advances in heterogeneous catalysts for the synthesis of cyclic carbonates from carbon dioxide

The novel heterogeneous catalysts are highly demanded to perform the cycloaddition reaction of carbon dioxide with epoxide to synthesize the cyclic carbonates. The heterogeneous catalysts are more preferred than homogeneous catalysts due to the easy post reaction separation, easy to recycle, high stability and cost effective nature. In this review, we have summarized the current research progress in heterogeneous catalysis for the cycloaddition of carbon dioxide (CO₂) to synthesis of cyclic carbonates. Recent advances in the design of the heterogeneous catalysts and the understanding to the role of catalysts in reaction process are summarized and discussed.     

Insights into electrochemical nitrogen reduction reaction mechanisms:Combined effect of single transition-metal and boron atom

Developing single-atom catalysts (SACs) for electrochemical devices is a frontier in energy conversion.The comparison of stability,activity and selectivity betw...     

Rational design of Cu-based electrocatalysts for electrochemical reduction of carbon dioxide

The recent development of Cu-based electrocatalysts for electrochemical reduction of carbon dioxide(CO_2) has attracted much attention due to their unique activity and selectivity compared to other metal catalysts. Particularly, Cu is the unique electrocatalyst for CO_2 electrochemical reduction with high selectivity to generate a variety of hydrocarbons. In this review, we mainly summarize the recent advances on the rational design of Cu nanostructures, the composition regulation of Cu-based alloys, and the exploitation of advanced supports for improving the catalytic activity and selectivity toward electrochemical reduction of CO_2. The special focus is to demonstrate how to enhance the activity and selectivity of Cubased electrocatalyst for CO_2 reduction. The perspectives and challenges for the development of Cu-based electrocatalysts are also addressed. We hope this review can provide timely and valuable insights into the design of advanced electrocatalytic materials for CO_2 electrochemical reduction.     

电化学氟化的新进展

电化学氟化是利用电极反应将氟直接引入有机或无机物的一种重要方法。有机物的电化学氟化方法有两种: 一是Simons于1941年发明的, 用镍作阳极, 在无水氟化氢溶液中, 电解制备全氟化合物的方法。此方法在近年来有不少改进。另一是1970年Rozhkov提出的, 以有机溶剂(如含Et3N.3HF的MeCN)为介质, 在铂阳极上,氧化得到单氟化产物的方法。本文全面地综述了这两种方法, 并着重于最新民发展。