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Investigation of Sulfur-Tolerant Catalysts for Selective Synthesis
of Hydrocarbon Liquids from Coal-Derived Gases
Final Technical Progress Report For Period September 19, 1979 to October 22, 1984

Bartholomew, Calvin H.

Brigham Young University

In this pdf format, this document has 66 pages and is 2.6MB

Table of Contents

Foreward iii
List of Tables v
List of Figures v
Abstract viii
 

I

Objectives and Scope

 1
 

A

Background

 1

B

Objectives

 1

C

Technical Approach

 2

II

Executive Summary

 7

III

Detailed Description of Technical Progress

 9
 

A

Task 1: Catalyst Preparation and Characterization

 9

B

Task 2: Activity/Selectivity Properties

 22

C

Task 3: In Situ H2S Poisoning Measurements

 35

D

Technical Communications and Miscellaneous Accomplishments

 39

IV

Conclusions

 51

V

References

 52
 
LIST OF TABLES  
1 Catalyst Preparation Plans (Task 1) 3
2 Experimental Plan 4
3 Summary of Catalysts Prepared 10
4 H2, CO, CO2 Adsorption Uptakes of Cobalt and Iron Catalysts After 36 hours of reduction 11
5 Chemisorption Data for Cobalt and Iron Boride Catalysts 13
6

Dispersion and Phase Analysis of K-Promoted Fe/SiO2

Catalysts		 21
7 CO Turnover Numbers for Supported Iron and Cobalt Catalysts 23
8 CO Turnover Numbers for Supported Iron and Cobalt Catalysts 23
9 Activities and Activation Energies for Unpromoted and Boron Promoted Cobalt and Iron Catalyst 25
10 Product Selectivities for Iron Boride Catalysts at 498 K and Cobalt Boride Catalysts at 483 K 26
11 Effect of Support on Fe Catalyst Activity  (2/1 H2/CO 1 atm, 498 K) 28
12 The Effect of Support on Selectivity of Fe Catalysts (2/1 H2/CO, 1 atm, 498 K) 29
13 Effects of K-level and Calcination Temperature on the CO Hydrogenation Activity of Fe/K/SiO2 (H2/CO=2, 1 atm, 523 K) 30
14 Effects of Potassium level and Calcination Temperature on Selectivity of K-Promoted Fe/SiO2 Catalysts (H2/CO=2, 1 atm) 31
15 Deactivation Rate Parameters for In Situ H2S Poisoning  40
16 Publications in Connection with this contract 42
17 Technical Meeting, Papers, and Presentations in Connection with this contract  43
18 Laboratories Visited by the Principal Investigator During Contract Period 45
19 Visitors and Speakers, BYU Catalysis Laboratory During Contract Period 47
20 Students Supported by Contract 50
 
LIST OF FIGURES  
1 Temperature programmed desorption spectra of H2 from 15% Fe/SiO2 (dried at 60-80ºC prior to reduction) as a function of temperature 15
2 Temperature-programmed desorption spectra of H2 from 15% Fe/SiO2 (dried at 100ºC) as a function of temperature 16
3 Temperature programmed spectra of H2 from 15% Fe/SiO2 (predried at 373 K) as a function of adsorption temperature 17
4 Temperature-programmed desorption of H2 from 15% Fe/3% K/SiO2 (calcined at 473 K) as a function of adsorption temperatures 18
5 Moeessbauer Spectra of Unsupported Iron Boride at Different States of Preparation 19
6 Moessbauer Spectra of reduced Fe/SiO2 and Fe/N/SiO2  20
7 Hydrocarbon Product Distribution and Schulz-Flory Plot. 15% Fe/SiO2 Fe/SiO2 (Calcined 473 K, H2/CO=2, 1 atm.) 32
8 Hydrocarbon Product Distribution and Schulz-Flory Plot. 15% Fe/3% K/SiO2 (Calcined 373 KO; 498 K, H2/CO=2, 1 atm.) 33
9 Hydrocarbon Product Distribution and Schulz-Flory Plot. 15% Fe/3% K/SiO2 (Calcined 473 K): 498 K, H2/CO = 2, 1 atm.)   34
10 Normalized Activity of Fe-S-102 at 0.6, 1.8, and 6.0 ppm H2S, 496-505 K, and H2/CO=2 as a Function of Sulfur to iron ratio 36
11 Normalized Activity of Fe-S-102 Fe-K-S-102, and Fe-100 at H2S Concentrations Below 2 ppm, H2/CO=2 37
12 Normalized Activity of Fe-B0101 at 0.5 and 8 ppm, 500 K, 38
13 Normalized Selectivity of Co-S-102 as a Function of Sulfur to Cobalt Ratio (6 ppm H2 S, 500 K, H2/CO = 2) 41