Abstract:A nanocomposite of Co/Co–Al2O3 nanosheets shows a high light-to-fuel efficiency and fuel production rate for photothermocatalytic CO2 reduction using CH4.
“…In addition, the reference samples of pure NiCo alloy nanoparticles with the Ni/Co molar ratios of 3.48 (labeled as Ni 3.48 Co), Ni nanoparticles supported on Co doped Al 2 O 3 nanosheets (labeled as Ni/Co–Al 2 O 3 ) were prepared. The reference samples of Ni nanoparticles supported on Al 2 O 3 nanosheets (labeled as Ni/Al 2 O 3 ) and Co nanoparticles supported on Al 2 O 3 nanosheets (labeled as Co/Al 2 O 3 ) were prepared according to the reported works [ 47,48 ] (see the Experimental Section in the Supporting Information).…”
Section: Resultsmentioning
confidence: 99%
“…[ 51 ] Metallic Co and Ni exist in Ni 1.60 Co/Co–Al 2 O 3 , consistent with the result of XRD and HRTEM. This is evidenced by weak peaks around 778.0 eV (Co), [ 48,51 ] and 851.8 eV (Ni). [ 47 ] Interestingly, as compared to the XPS peak around 852.6 eV of metallic Ni (e.g., in a reference sample of Ni/Al 2 O 3 , Supporting Information), [ 47,51 ] the peak of metallic Ni in Ni 1.60 Co/Co–Al 2 O 3 obviously shifts to 851.8 eV.…”
Section: Resultsmentioning
confidence: 99%
“…Recently, an approach of photothermocatalysis for CO 2 reduction by water, [ 33–35 ] hydrogen, [ 36–40 ] and methane [ 41–49 ] was developed. The approach is very efficient and promising as it well integrates low energy consumption of photocatalysis with high efficiency of thermocatalysis.…”
Section: Introductionmentioning
confidence: 99%
“…In the approach, photothermocatalytic CO 2 reduction by methane to produce carbon monoxide and hydrogen (CRM, CO 2 + CH 4 = 2CO + 2H 2 , Δ H 298 = 247 kJ mol −1 , usually referred to as dry reforming of methane) is very appealing and promising because it is able to achieve high r fuel and η at the same time. [ 44–48 ] Methane is utilized as reductant in photothermocatalytic CRM due to its abundance and low cost as major component of natural gas. Moreover, its products may be utilized as syngas to synthesize liquid fuels by industrial Fischer–Tropsch technology and acquire clean hydrogen fuel by industrial separation technology.…”
Section: Introductionmentioning
confidence: 99%
“…[ 41–49 ] Among the catalysts, nonprecious metal catalysts such as Ni and Co are appealing due to their earth abundance, low cost, and good catalytic activity. [ 43,45–48 ] However, unlike noble metal catalysts with good resistance to carbon deposition, nonprecious metal catalysts are prone to deactivation due to two side‐reactions of carbon deposition such as CO disproportionation (2CO = C + CO 2 , Δ H 298 = −171 kJ mol −1 ) and methane dissociation (CH 4 = C + 2H 2 , Δ H 298 = 75 kJ mol −1 ). The catalyst deactivation is major challenge for the practical application of photothermocatalytic CRM in greenhouse gas control and solar energy storage.…”
Unique nanocomposites of NiCo alloy nanoparticles with Ni/Co molar ratios of 1.86, 1.60, and 0.38 supported on Co‐doped Al2O3 nanosheets are prepared by a facile approach. Very high fuel production rates of CO (rCO) and H2 (rH2) (70.53 and 63.46 mmol min−1 g−1) and light‐to‐fuel efficiency (η, 29.7%) are achieved via photothermocatalytic CO2 reduction by methane (CRM) on Ni1.60Co/Co‐Al2O3 simply utilizing focused UV‐visible‐infrared (UV‐vis‐IR) illumination. Ni1.60Co/Co‐Al2O3 also demonstrates high rCO and rH2 values (50.99 and 39.72 mmol min−1 g−1) as well as high η value (26.3%) under λ > 560 nm focused vis‐IR illumination. The high photothermocatalytic activity is derived from the light‐driven thermocatalytic CRM. A novel photoactivation is found to substantially promote the light‐driven thermocatalytic CRM due to the apparent activation energy being considerably reduced upon illumination. It is found that the Ni/Co molar ratio in the NiCo/Co‐Al2O3 samples has an important effect on the photothermocatalytic durability. The samples of Ni1.60Co/Co‐Al2O3 and Ni1.86Co/Co‐Al2O3 with a higher Ni/Co molar ratio demonstrate excellent photothermocatalytic durability, while the Ni0.38Co/Co‐Al2O3 with a lower Ni/Co molar ratio has less durability. This is attributed to carbon deposition rate being significantly reduced on Ni1.60Co/Co‐Al2O3 and Ni1.86Co/Co‐Al2O3 as compared to its single metal counterparts.
“…In addition, the reference samples of pure NiCo alloy nanoparticles with the Ni/Co molar ratios of 3.48 (labeled as Ni 3.48 Co), Ni nanoparticles supported on Co doped Al 2 O 3 nanosheets (labeled as Ni/Co–Al 2 O 3 ) were prepared. The reference samples of Ni nanoparticles supported on Al 2 O 3 nanosheets (labeled as Ni/Al 2 O 3 ) and Co nanoparticles supported on Al 2 O 3 nanosheets (labeled as Co/Al 2 O 3 ) were prepared according to the reported works [ 47,48 ] (see the Experimental Section in the Supporting Information).…”
Section: Resultsmentioning
confidence: 99%
“…[ 51 ] Metallic Co and Ni exist in Ni 1.60 Co/Co–Al 2 O 3 , consistent with the result of XRD and HRTEM. This is evidenced by weak peaks around 778.0 eV (Co), [ 48,51 ] and 851.8 eV (Ni). [ 47 ] Interestingly, as compared to the XPS peak around 852.6 eV of metallic Ni (e.g., in a reference sample of Ni/Al 2 O 3 , Supporting Information), [ 47,51 ] the peak of metallic Ni in Ni 1.60 Co/Co–Al 2 O 3 obviously shifts to 851.8 eV.…”
Section: Resultsmentioning
confidence: 99%
“…Recently, an approach of photothermocatalysis for CO 2 reduction by water, [ 33–35 ] hydrogen, [ 36–40 ] and methane [ 41–49 ] was developed. The approach is very efficient and promising as it well integrates low energy consumption of photocatalysis with high efficiency of thermocatalysis.…”
Section: Introductionmentioning
confidence: 99%
“…In the approach, photothermocatalytic CO 2 reduction by methane to produce carbon monoxide and hydrogen (CRM, CO 2 + CH 4 = 2CO + 2H 2 , Δ H 298 = 247 kJ mol −1 , usually referred to as dry reforming of methane) is very appealing and promising because it is able to achieve high r fuel and η at the same time. [ 44–48 ] Methane is utilized as reductant in photothermocatalytic CRM due to its abundance and low cost as major component of natural gas. Moreover, its products may be utilized as syngas to synthesize liquid fuels by industrial Fischer–Tropsch technology and acquire clean hydrogen fuel by industrial separation technology.…”
Section: Introductionmentioning
confidence: 99%
“…[ 41–49 ] Among the catalysts, nonprecious metal catalysts such as Ni and Co are appealing due to their earth abundance, low cost, and good catalytic activity. [ 43,45–48 ] However, unlike noble metal catalysts with good resistance to carbon deposition, nonprecious metal catalysts are prone to deactivation due to two side‐reactions of carbon deposition such as CO disproportionation (2CO = C + CO 2 , Δ H 298 = −171 kJ mol −1 ) and methane dissociation (CH 4 = C + 2H 2 , Δ H 298 = 75 kJ mol −1 ). The catalyst deactivation is major challenge for the practical application of photothermocatalytic CRM in greenhouse gas control and solar energy storage.…”
Unique nanocomposites of NiCo alloy nanoparticles with Ni/Co molar ratios of 1.86, 1.60, and 0.38 supported on Co‐doped Al2O3 nanosheets are prepared by a facile approach. Very high fuel production rates of CO (rCO) and H2 (rH2) (70.53 and 63.46 mmol min−1 g−1) and light‐to‐fuel efficiency (η, 29.7%) are achieved via photothermocatalytic CO2 reduction by methane (CRM) on Ni1.60Co/Co‐Al2O3 simply utilizing focused UV‐visible‐infrared (UV‐vis‐IR) illumination. Ni1.60Co/Co‐Al2O3 also demonstrates high rCO and rH2 values (50.99 and 39.72 mmol min−1 g−1) as well as high η value (26.3%) under λ > 560 nm focused vis‐IR illumination. The high photothermocatalytic activity is derived from the light‐driven thermocatalytic CRM. A novel photoactivation is found to substantially promote the light‐driven thermocatalytic CRM due to the apparent activation energy being considerably reduced upon illumination. It is found that the Ni/Co molar ratio in the NiCo/Co‐Al2O3 samples has an important effect on the photothermocatalytic durability. The samples of Ni1.60Co/Co‐Al2O3 and Ni1.86Co/Co‐Al2O3 with a higher Ni/Co molar ratio demonstrate excellent photothermocatalytic durability, while the Ni0.38Co/Co‐Al2O3 with a lower Ni/Co molar ratio has less durability. This is attributed to carbon deposition rate being significantly reduced on Ni1.60Co/Co‐Al2O3 and Ni1.86Co/Co‐Al2O3 as compared to its single metal counterparts.
Global warming and the energy shortage due to the burning of fossil fuels are two major challenges. A strategy of light-driven catalytic dry reforming of methane (DRM) using inexhaustible solar energy has provided an effective approach to tackle these challenges. Loaded metallic Ni nanoparticles have been identified as promising catalysts as alternatives to noble metals for DRM. However, they suffer from quick deactivation caused by severe coking due to thermodynamically inevitable side-reactions. Herein, a unique nickel half-metal catalyst of monolayer nickel clusters stabilized by alumina is reported, with 100% atomic utilization efficiency and extraordinary catalytic performance for light-driven DRM, dramatically different from its counterpart of conventional metallic Ni nanoparticles. It has extremely high specific H 2 and CO production rates of 8572.96 and 9614.26 mmol min −1 gNi −1 , more than one order of magnitude higher than those of Ni nanoparticles. No detectable coke is formed due to the alteration of kinetic processes for DRM, resulting in the inhibition of coke deposition. It is discovered that light not only significantly enhances catalytic activity, but also enables quick thermocatalytic deactivation to be durable due to the oxidation of carbon species and the desorption of strongly adsorbed CO 2 and CO being dramatically promoted by light.
The ability to use the full solar spectrum energy in photocatalytic processes for environmental remediation and energy production has attracted worldwide attention. Efficient harvesting of near‐infrared (NIR) photons, especially in the wavelength range beyond 800 nm, is one of the main driving forces in photocatalytic research. The design of appropriate photocatalytic systems for wide‐range light‐harvesting from the UV to NIR regions is a promising method of maximizing the efficiency of solar energy utilization. This review comprehensively summarizes the recent progress in full‐solar‐light‐driven photocatalytic systems, including several strategies to harness NIR light and thermal energy. The corresponding photocatalytic mechanisms and design of binary or ternary heterogeneous systems are discussed in detail. Moreover, future perspectives and challenges are presented to inspire the development of further innovations in full‐solar‐light‐driven photocatalysis.
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