Trash to treasure: Use flue gas SO2 to produce H2 via a photoelectrochemical process

Abstract Sulfur dioxide (SO2), emitting from power plant and factories, has been one of the major atmospheric pollutants and causes lots of harmful environmental issues. Although some mature desulfurization technologies are available, a more economic or even profitable approach for flue gas desulfurization is greatly desirable. Herein, we report SO2 can be efficiently recycled to produce H2 via a photoelectrochemical (PEC) water splitting process based on Mo-doped BiVO4 inverse opals. Via this process, the SO2 removal rate is higher than 97%, the absorbed SO2 can act as a sacrifice reagent to produce H2 in the PEC water splitting. With the design of the highly ordered porous structure, the generation rate of H2 is improved by tens of times. Via the proposed process, the SO2 released (0.03 kg) from coal power plant for a generation of 1 kW h electricity can be recycled to produce around 10 L H2. By combining with ammonia-based desulfurization technology, the production of H2 can greatly reduce the cost of ammonia-based desulfurization technology and make it profitable.

[1]  Sang J. Chung,et al.  Novel process for simultaneous removal of NO(x) and SO2 from simulated flue gas by using a sustainable Ag(I)/Ag(II) redox mediator. , 2008, Environmental science & technology.

[2]  Shuxin Ouyang,et al.  Nano‐photocatalytic Materials: Possibilities and Challenges , 2012, Advanced materials.

[3]  Kyoung-Shin Choi,et al.  A new electrochemical synthesis route for a BiOI electrode and its conversion to a highly efficient porous BiVO4 photoanode for solar water oxidation , 2012 .

[4]  Li Wang,et al.  Hollow Cobalt-Based Bimetallic Sulfide Polyhedra for Efficient All-pH-Value Electrochemical and Photocatalytic Hydrogen Evolution. , 2016, Journal of the American Chemical Society.

[5]  Can Li,et al.  Importance of the relationship between surface phases and photocatalytic activity of TiO2. , 2008, Angewandte Chemie.

[6]  Hui Li,et al.  High-index faceted Ni3S2 nanosheet arrays as highly active and ultrastable electrocatalysts for water splitting. , 2015, Journal of the American Chemical Society.

[7]  A. T-Raissi,et al.  Hydrogen production via photolytic oxidation of aqueous sodium sulfite solutions. , 2010, Environmental science & technology.

[8]  Shu Tao,et al.  Sulfur dioxide emissions from combustion in china: from 1990 to 2007. , 2011, Environmental science & technology.

[9]  Ling Zhang,et al.  Solar Light Driven Pure Water Splitting on Quantum Sized BiVO4 without any Cocatalyst , 2014 .

[10]  Liang‐Nian He,et al.  Highly efficient SO2 absorption/activation and subsequent utilization by polyethylene glycol-functionalized Lewis basic ionic liquids. , 2012, Physical chemistry chemical physics : PCCP.

[11]  Liang‐Nian He,et al.  Highly efficient SO₂ absorption and its subsequent utilization by weak base/polyethylene glycol binary system. , 2013, Environmental science & technology.

[12]  J. Baumberg,et al.  Plasmonic Enhancement in BiVO4 Photonic Crystals for Efficient Water Splitting , 2014, Small.

[13]  Gang Wu,et al.  Accelerated reduction in SO₂ emissions from the U.S. power sector triggered by changing prices of natural gas. , 2012, Environmental science & technology.

[14]  Hanyang Gao,et al.  Novel process of simultaneous removal of SO2 and NO2 by sodium humate solution. , 2010, Environmental science & technology.

[15]  H. Fu,et al.  Removal of SO2 on a nanoporous photoelectrode with simultaneous H2 production. , 2017 .

[16]  Jingjing Liu,et al.  Hydrolysis of Sulfur Dioxide in Small Clusters of Sulfuric Acid: Mechanistic and Kinetic Study. , 2015, Environmental science & technology.

[17]  M. Grutzeck,et al.  The Adsorption of SO2 by Zeolites Synthesized from Fly Ash , 1999 .

[18]  S. Marinescu,et al.  Efficient Electrochemical and Photoelectrochemical H2 Production from Water by a Cobalt Dithiolene One-Dimensional Metal-Organic Surface. , 2015, Journal of the American Chemical Society.

[19]  E. López-Salinas,et al.  SOx removal by calcined MgAlFe hydrotalcite-like materials: effect of the chemical composition and the cerium incorporation method. , 2005, Environmental science & technology.

[20]  Takashi Hisatomi,et al.  Ultrastable low-bias water splitting photoanodes via photocorrosion inhibition and in situ catalyst regeneration , 2016, Nature Energy.

[21]  G. Stucky,et al.  Anisotropic Growth of TiO2 onto Gold Nanorods for Plasmon-Enhanced Hydrogen Production from Water Reduction. , 2016, Journal of the American Chemical Society.

[22]  Jinwon Park,et al.  Adsorption characteristics of SO2 on activated carbon prepared from coconut shell with potassium hydroxide activation. , 2002, Environmental science & technology.

[23]  T. Bandosz,et al.  Adsorption of SO2 on sewage sludge-derived materials. , 2001, Environmental science & technology.

[24]  Gunawan,et al.  Pt/In2S3/CdS/Cu2ZnSnS4 Thin Film as an Efficient and Stable Photocathode for Water Reduction under Sunlight Radiation. , 2015, Journal of the American Chemical Society.

[25]  Charles Q. Jia,et al.  Simultaneous Sulfur Dioxide Absorption and Hydrogen Sulfide Generation in an Aqueous Solution of Sodium Sulfide , 1996 .

[26]  Zifeng Lu,et al.  Ozone monitoring instrument observations of interannual increases in SO2 emissions from Indian coal-fired power plants during 2005-2012. , 2013, Environmental science & technology.

[27]  Can Li,et al.  Enhancement of photocatalytic H2 evolution on CdS by loading MoS2 as Cocatalyst under visible light irradiation. , 2008, Journal of the American Chemical Society.

[28]  Xuchang Xu,et al.  Simultaneous removal of SO2 and trace SeO2 from flue gas: effect of product layer on mass transfer. , 2006, Environmental science & technology.

[29]  R. Schlögl,et al.  Molecular Insight in Structure and Activity of Highly Efficient, Low-Ir Ir-Ni Oxide Catalysts for Electrochemical Water Splitting (OER). , 2015, Journal of the American Chemical Society.

[30]  Hong Liu,et al.  A new concept of desulfurization: the electrochemically driven and green conversion of SO2 to NaHSO4 in aqueous solution. , 2008, Environmental science & technology.

[31]  Yang Xu,et al.  Photoelectrodes based upon Mo:BiVO4 inverse opals for photoelectrochemical water splitting. , 2014, ACS nano.

[32]  K. Domen,et al.  Mg-Zr Cosubstituted Ta3N5 Photoanode for Lower-Onset-Potential Solar-Driven Photoelectrochemical Water Splitting. , 2015, Journal of the American Chemical Society.

[33]  H. Sohn,et al.  A new process for converting SO2 to sulfur without generating secondary pollutants through reactions involving CaS and CaSO4. , 2002, Environmental science & technology.

[34]  David Allen,et al.  Dynamic Management of NOx and SO2 Emissions in the Texas and Mid-Atlantic Electric Power Systems and Implications for Air Quality. , 2016, Environmental science & technology.